首页 > 最新文献

Journal of Membrane Science最新文献

英文 中文
PPS-reinforced poly(terphenylene) anion-exchange membranes with different quaternary ammonium groups for use in water electrolysers 用于水电解槽的具有不同季铵基团的 PPS 增强聚(三联苯)阴离子交换膜
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-15 DOI: 10.1016/j.memsci.2024.123335
The nature, concentration and spatial distribution of quaternary ammonium (QA) groups is instrumental for the performance of anion exchange membranes, primarily by augmenting the ion exchange capacity (IEC). This study compares a series of poly(meta-terphenylene)-based ion exchange membranes (mTPN), which vary in the attached quaternary ammonium group. The IEC of the membranes is 1.97, 2.20 and 3.70 mmol OH g−1 for membranes functionalized with 1,4-diazabicyclo[2.2.2]octane (DABCO), trimethylamine (TMA), and methylated DABCO (DABCO-Me), respectively. The latter is obtained by methylation of the DABCO-functionalized membrane.
To control swelling, all membranes are reinforced with a poly(phenylene sulfide) (PPS) fiber mat. The highest conductivity, achieved by PPS/mTPN/DABCO-Me, is 140 mS cm−1 in 1 M KOH and 237 mS cm−1 in 4 M KOH. An alkaline stability test over 2 months revealed that membranes with TMA and DABCO have a stable in-plane conductivity, measured in pure water, while the membrane with DABCO-Me showed a strongly increased resistance. On the other hand, a 1 month stability test showed that the through-plane conductivity of the membrane with DABCO-Me in 1 M KOH hardly changed. This indicates that conductivity by absorbed KOH solution is more relevant than the conductivity provided by the quaternary ammonium groups, and promises stable operation in the electrolyser. This is supported by an electrolyser test, where a stable voltage of 1.9 V at 0.25 A cm−2 was achieved, with no observed change in membrane resistance over a test duration of 100 h (60 °C, 4 M KOH, PGM-free catalyst).
季铵(QA)基团的性质、浓度和空间分布对阴离子交换膜的性能至关重要,主要是通过增强离子交换能力(IEC)。本研究比较了一系列基于聚(偏三联苯)的离子交换膜(mTPN),这些膜所附的季铵基团各不相同。用 1,4-二氮杂双环[2.2.2]辛烷(DABCO)、三甲胺(TMA)和甲基化 DABCO(DABCO-Me)功能化的膜的 IEC 分别为 1.97、2.20 和 3.70 mmol OH- g-1。为了控制膨胀,所有膜都使用聚苯硫醚(PPS)纤维毡进行增强。PPS/mTPN/DABCO-Me 的最高电导率在 1 M KOH 中为 140 mS cm-1,在 4 M KOH 中为 237 mS cm-1。为期 2 个月的碱性稳定性测试表明,在纯水中测量,含有 TMA 和 DABCO 的膜具有稳定的面内电导率,而含有 DABCO-Me 的膜则显示出强烈的电阻增加。另一方面,1 个月的稳定性测试表明,含有 DABCO-Me 的膜在 1 M KOH 中的面内电导率几乎没有变化。这表明,吸收 KOH 溶液的导电性比季铵基团提供的导电性更重要,并有望在电解槽中稳定运行。电解槽测试也证明了这一点,在 0.25 A cm-2 的条件下,测试电压稳定在 1.9 V,在 100 小时的测试时间内(60 °C,4 M KOH,不含 PGM 的催化剂),没有观察到膜电阻的变化。
{"title":"PPS-reinforced poly(terphenylene) anion-exchange membranes with different quaternary ammonium groups for use in water electrolysers","authors":"","doi":"10.1016/j.memsci.2024.123335","DOIUrl":"10.1016/j.memsci.2024.123335","url":null,"abstract":"<div><div>The nature, concentration and spatial distribution of quaternary ammonium (QA) groups is instrumental for the performance of anion exchange membranes, primarily by augmenting the ion exchange capacity (IEC). This study compares a series of poly(<em>meta</em>-terphenylene)-based ion exchange membranes (mTPN), which vary in the attached quaternary ammonium group. The IEC of the membranes is 1.97, 2.20 and 3.70 mmol OH<sup>−</sup> g<sup>−1</sup> for membranes functionalized with 1,4-diazabicyclo[2.2.2]octane (DABCO), trimethylamine (TMA), and methylated DABCO (DABCO-Me), respectively. The latter is obtained by methylation of the DABCO-functionalized membrane.</div><div>To control swelling, all membranes are reinforced with a poly(phenylene sulfide) (PPS) fiber mat. The highest conductivity, achieved by PPS/mTPN/DABCO-Me, is 140 mS cm<sup>−1</sup> in 1 M KOH and 237 mS cm<sup>−1</sup> in 4 M KOH. An alkaline stability test over 2 months revealed that membranes with TMA and DABCO have a stable in-plane conductivity, measured in pure water, while the membrane with DABCO-Me showed a strongly increased resistance. On the other hand, a 1 month stability test showed that the through-plane conductivity of the membrane with DABCO-Me in 1 M KOH hardly changed. This indicates that conductivity by absorbed KOH solution is more relevant than the conductivity provided by the quaternary ammonium groups, and promises stable operation in the electrolyser. This is supported by an electrolyser test, where a stable voltage of 1.9 V at 0.25 A cm<sup>−2</sup> was achieved, with no observed change in membrane resistance over a test duration of 100 h (60 °C, 4 M KOH, PGM-free catalyst).</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0376738824009293/pdfft?md5=6a8ecda3208ee7ef9db0e077bc957b6e&pid=1-s2.0-S0376738824009293-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142316079","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Charge mediated nano-filtration for recovering sinapic acid from a mustard bran hydrolysate 电荷介导纳米过滤从芥子麸水解物中回收山奈酸
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-14 DOI: 10.1016/j.memsci.2024.123333

The recovery of valuable chemicals, such as sinapic acid, from enzymatic hydrolysates is essential to enabling a sustainable biorefinery. In this study, we designed a system to recover sinapic acid produced chemo-enzymatically from waste mustard bran. The process involves sequential separation, beginning with size partitioning using ultrafiltration for enzyme removal and recovery, followed by charge-mediated size partitioning via nanofiltration to isolate sinapic acid from other extracts. Four polyethersulfone (PES) ultrafiltration membranes with molecular weight cut-offs (MWCOs) of 5000 and 10 000 Da and maximum allowable working pressures (MAWPs) of 3 and 10 bar were screened for their effectiveness in removing Bovine Serum Albumin (BSA) as a model compound. Subsequently, these membranes were applied to recover the feruloyl esterase enzyme. The membrane with an MWCO of 5000 Da and an MAWP of 10 bar achieved 97.93 % enzyme recovery with a permeate flow rate of 31.4 L/h/m2 at 6 bar. Next, we evaluated the effects of zeta potential interactions on the preferential rejection of sinapic acid using various nanofiltration membranes with potentially charged surfaces, including polyimide, silicon-based thin film composite, and polypiperazine amide membranes with MWCOs ranging from 150 to 600 Da. The polypiperazine amide membrane demonstrated the highest recovery of sinapic acid, achieving 86 % recovery from a model solution and 64 % recovery from mustard bran hydrolysate. Compositional analysis of the permeate confirmed that the rejection rate (R) is influenced primarily by the pKa rather than molecular size, following the trend: sinapic acid (pKa = 4.58; 224.2 Da; R = 64.0 %), acetic acid (pKa = 4.76; 60.1 Da; R = 23.8 %), xylose (pKa = 12.15; 150.1 Da; R = 13.7 %), glucose (pKa = 12.28; 180.2 Da; R = 8.7 %), and arabinose (pKa = 12.34; 150.1 Da; R = 8.5 %). The zeta potential interactions across nanofiltration membranes enhanced sinapic acid recovery from the mustard bran hydrolysate, hence, charge mediation significantly influenced the membrane separation of these complex mixtures with varying pKa values.

从酶水解物中回收有价值的化学物质(如山奈酸)对于实现可持续生物精炼至关重要。在这项研究中,我们设计了一种从废弃芥菜麸中回收化学酶法生产的山奈酸的系统。该工艺包括顺序分离,首先使用超滤进行粒度分区以去除和回收酶,然后通过纳滤进行电荷介导的粒度分区,从其他提取物中分离出山奈酸。筛选了四种聚醚砜(PES)超滤膜,它们的分子量截断点(MWCOs)分别为 5000 和 10 000 Da,最大允许工作压力(MAWPs)分别为 3 和 10 bar,以检测它们去除作为模型化合物的牛血清白蛋白(BSA)的效果。随后,这些膜被用于回收阿魏酰酯酶。截留分子量为 5000 Da、MAWP 为 10 bar 的膜在 6 bar 条件下的渗透流速为 31.4 L/h/m2,酶回收率达到 97.93%。接下来,我们使用各种表面可能带电的纳滤膜,包括截留分子量在 150 到 600 Da 之间的聚酰亚胺膜、硅基薄膜复合膜和聚哌嗪酰胺膜,评估了 zeta 电位相互作用对优先截留正那酸的影响。聚哌嗪酰胺膜的山奈酸回收率最高,从模型溶液中的回收率达到 86%,从芥子麸水解物中的回收率达到 64%。渗透物的成分分析证实,排斥率(R)主要受 pKa 而不是分子大小的影响,其趋势如下:正己酸(pKa = 4.58;224.2 Da; R = 64.0 %)、乙酸(pKa = 4.76; 60.1 Da; R = 23.8 %)、木糖(pKa = 12.15; 150.1 Da; R = 13.7 %)、葡萄糖(pKa = 12.28; 180.2 Da; R = 8.7 %)和阿拉伯糖(pKa = 12.34; 150.1 Da; R = 8.5 %)。纳滤膜上的 zeta 电位相互作用提高了芥子麸水解物中的山奈酸回收率,因此,电荷调解对这些具有不同 pKa 值的复杂混合物的膜分离有显著影响。
{"title":"Charge mediated nano-filtration for recovering sinapic acid from a mustard bran hydrolysate","authors":"","doi":"10.1016/j.memsci.2024.123333","DOIUrl":"10.1016/j.memsci.2024.123333","url":null,"abstract":"<div><p>The recovery of valuable chemicals, such as sinapic acid, from enzymatic hydrolysates is essential to enabling a sustainable biorefinery. In this study, we designed a system to recover sinapic acid produced chemo-enzymatically from waste mustard bran. The process involves sequential separation, beginning with size partitioning using ultrafiltration for enzyme removal and recovery, followed by charge-mediated size partitioning via nanofiltration to isolate sinapic acid from other extracts. Four polyethersulfone (PES) ultrafiltration membranes with molecular weight cut-offs (MWCOs) of 5000 and 10 000 Da and maximum allowable working pressures (MAWPs) of 3 and 10 bar were screened for their effectiveness in removing Bovine Serum Albumin (BSA) as a model compound. Subsequently, these membranes were applied to recover the feruloyl esterase enzyme. The membrane with an MWCO of 5000 Da and an MAWP of 10 bar achieved 97.93 % enzyme recovery with a permeate flow rate of 31.4 L/h/m<sup>2</sup> at 6 bar. Next, we evaluated the effects of zeta potential interactions on the preferential rejection of sinapic acid using various nanofiltration membranes with potentially charged surfaces, including polyimide, silicon-based thin film composite, and polypiperazine amide membranes with MWCOs ranging from 150 to 600 Da. The polypiperazine amide membrane demonstrated the highest recovery of sinapic acid, achieving 86 % recovery from a model solution and 64 % recovery from mustard bran hydrolysate. Compositional analysis of the permeate confirmed that the rejection rate (R) is influenced primarily by the pKa rather than molecular size, following the trend: sinapic acid (pKa = 4.58; 224.2 Da; R = 64.0 %), acetic acid (pKa = 4.76; 60.1 Da; R = 23.8 %), xylose (pKa = 12.15; 150.1 Da; R = 13.7 %), glucose (pKa = 12.28; 180.2 Da; R = 8.7 %), and arabinose (pKa = 12.34; 150.1 Da; R = 8.5 %). The zeta potential interactions across nanofiltration membranes enhanced sinapic acid recovery from the mustard bran hydrolysate, hence, charge mediation significantly influenced the membrane separation of these complex mixtures with varying pKa values.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142271793","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Permeability of gas molecules through sub-nanometer nitrogen-terminated porous graphene membranes: A DFT study 气体分子通过亚纳米氮端多孔石墨烯膜的渗透性:DFT 研究
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-13 DOI: 10.1016/j.memsci.2024.123329

We present a systematic theoretical investigation of gas permeability through single-layer nanoporous graphene membranes with N-terminated (pyridinic and mixed pyridinic/pyrrolic) pores for He, H2, N2, O2, CO, CO2, H2O, and CH4. Our study is based on density functional theory transition-state calculations and the kinetic theory of gasses. We systematically evaluate pores of varying sizes and shapes up to 5.7 Å in diameter. According to our findings, membranes with pores in the size regime (4.5 Å - 5.0 Å) may exhibit industrially acceptable permeance to several gas molecules and advanced selectivity. Notably, we found that, among a few others, a pore with the same topological features at the pore boundary as those of the characteristic pore of g-C3N4 carbon nitride, is particularly promising. In addition, membranes with larger pores, 5.5 Å - 5.7 Å, can effectively separate CH4 from the other molecules. Our findings support the advanced potential of single-layer graphene membranes with nitrogen-terminated sub-nanometer pores, for gas separation applications.

我们对具有 N 端(吡啶和吡啶/吡咯混合)孔隙的单层纳米多孔石墨烯膜对 He、H2、N2、O2、CO、CO2、H2O 和 CH4 的气体渗透性进行了系统的理论研究。我们的研究基于密度泛函理论过渡态计算和气体动力学理论。我们系统地评估了直径达 5.7 Å 的不同大小和形状的孔。根据我们的研究结果,孔径在 4.5 Å - 5.0 Å 范围内的膜可以表现出工业上可接受的对多种气体分子的渗透性和高级选择性。值得注意的是,我们发现孔边界拓扑特征与 g-C3N4 氮化碳特征孔相同的孔尤其具有发展前景。此外,孔隙较大(5.5 Å - 5.7 Å)的膜能有效地将 CH4 与其他分子分离。我们的研究结果支持了氮封端亚纳米孔隙的单层石墨烯膜在气体分离应用中的先进潜力。
{"title":"Permeability of gas molecules through sub-nanometer nitrogen-terminated porous graphene membranes: A DFT study","authors":"","doi":"10.1016/j.memsci.2024.123329","DOIUrl":"10.1016/j.memsci.2024.123329","url":null,"abstract":"<div><p>We present a systematic theoretical investigation of gas permeability through single-layer nanoporous graphene membranes with N-terminated (pyridinic and mixed pyridinic/pyrrolic) pores for He, H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, N<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, CO, CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O, and CH<span><math><msub><mrow></mrow><mrow><mn>4</mn></mrow></msub></math></span>. Our study is based on density functional theory transition-state calculations and the kinetic theory of gasses. We systematically evaluate pores of varying sizes and shapes up to 5.7 Å in diameter. According to our findings, membranes with pores in the size regime (4.5 Å - 5.0 Å) may exhibit industrially acceptable permeance to several gas molecules and advanced selectivity. Notably, we found that, among a few others, a pore with the same topological features at the pore boundary as those of the characteristic pore of g-C<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span>N<span><math><msub><mrow></mrow><mrow><mn>4</mn></mrow></msub></math></span> carbon nitride, is particularly promising. In addition, membranes with larger pores, <span><math><mo>∼</mo></math></span>5.5 Å - 5.7 Å, can effectively separate CH<span><math><msub><mrow></mrow><mrow><mn>4</mn></mrow></msub></math></span> from the other molecules. Our findings support the advanced potential of single-layer graphene membranes with nitrogen-terminated sub-nanometer pores, for gas separation applications.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142271795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Construction of ion transport channels in cation exchange membranes by embedding MXene with dual regulation strategy for electrodialysis 通过嵌入 MXene 在阳离子交换膜中构建离子传输通道,采用双重调控策略进行电渗析
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-13 DOI: 10.1016/j.memsci.2024.123322
Ion exchange membranes (IEMs) have a wider application in water purification, electrolytic process, and ion separation. The improvement of IEMs performance through sulfonation treatment is limited, which seriously affects their application. Therefore, the incorporation of two-dimensional MXene can serve as a new breakthrough for exploration. However, the size of MXene nanosheets has not received significant attention in the studies of preparing composite membranes. The focus of this work was to explore the effect of MXene nanosheets on IEMs from the perspective of nanosheet size. Specifically, by adjusting the sizes of MXene nanosheets using simple sonication treatment, the continuous ion transport channels were constructed by connecting non-conductive regions in the matrix owing to uniform distribution and abundant hydroxyl functional groups of MXene nanosheets. Afterwards, content regulation was supplemented to increase the distribution density of negatively charged MXene nanosheets in the matrix, thereby further increasing the migration rate of ions. Through this special synergistic regulatory effect, the performance of the composite membrane was maximally improved. Additionally, SPM membrane achieved better IEC and permeability, as well as lower membrane area resistance compared to pristine SPSF membrane. When applied to the ED process, SPM1.0%-1.5h membrane revealed higher desalination performance (90.4 %) and current efficiency (104.2 %) compared to pristine SPSF membrane (86.6 % and 99.7 %, respectively).
离子交换膜(IEM)在水净化、电解过程和离子分离方面有着广泛的应用。通过磺化处理提高离子交换膜性能的方法有限,这严重影响了离子交换膜的应用。因此,二维 MXene 的加入可以作为一个新的突破口进行探索。然而,在制备复合膜的研究中,MXene 纳米片的尺寸并未受到重视。这项工作的重点是从纳米片尺寸的角度探讨 MXene 纳米片对 IEM 的影响。具体来说,通过简单的超声处理调节 MXene 纳米片的尺寸,由于 MXene 纳米片分布均匀且具有丰富的羟基官能团,因此可以通过连接基质中的非导电区域构建连续的离子传输通道。然后,再辅以含量调节,增加带负电的 MXene 纳米片在基质中的分布密度,从而进一步提高离子迁移率。通过这种特殊的协同调节作用,复合膜的性能得到了最大程度的提高。此外,与原始的 SPSF 膜相比,SPM 膜的 IEC 和渗透性更好,膜面积电阻更低。与原始的 SPSF 膜(分别为 86.6% 和 99.7%)相比,SPM1.0%-1.5h 膜在 ED 过程中显示出更高的脱盐性能(90.4%)和电流效率(104.2%)。
{"title":"Construction of ion transport channels in cation exchange membranes by embedding MXene with dual regulation strategy for electrodialysis","authors":"","doi":"10.1016/j.memsci.2024.123322","DOIUrl":"10.1016/j.memsci.2024.123322","url":null,"abstract":"<div><div>Ion exchange membranes (IEMs) have a wider application in water purification, electrolytic process, and ion separation. The improvement of IEMs performance through sulfonation treatment is limited, which seriously affects their application. Therefore, the incorporation of two-dimensional MXene can serve as a new breakthrough for exploration. However, the size of MXene nanosheets has not received significant attention in the studies of preparing composite membranes. The focus of this work was to explore the effect of MXene nanosheets on IEMs from the perspective of nanosheet size. Specifically, by adjusting the sizes of MXene nanosheets using simple sonication treatment, the continuous ion transport channels were constructed by connecting non-conductive regions in the matrix owing to uniform distribution and abundant hydroxyl functional groups of MXene nanosheets. Afterwards, content regulation was supplemented to increase the distribution density of negatively charged MXene nanosheets in the matrix, thereby further increasing the migration rate of ions. Through this special synergistic regulatory effect, the performance of the composite membrane was maximally improved. Additionally, SPM membrane achieved better IEC and permeability, as well as lower membrane area resistance compared to pristine SPSF membrane. When applied to the ED process, SPM1.0%-1.5h membrane revealed higher desalination performance (90.4 %) and current efficiency (104.2 %) compared to pristine SPSF membrane (86.6 % and 99.7 %, respectively).</div></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142316005","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effect of porous irregular ZrO2 nanoparticles on the performance of alkaline water electrolysis composite separator membranes under complex conditions 多孔不规则 ZrO2 纳米粒子对复杂条件下碱性水电解复合分离膜性能的影响
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-13 DOI: 10.1016/j.memsci.2024.123332

Developing composite separator membranes with low area resistance, high bubble point pressure, and long-term safety and stability is crucial for alkaline water electrolysis for hydrogen production as a key component of electrolyzer systems. In this study, PPS mesh fabric reinforced PSF@ZrO2 composite separator membranes were successfully prepared using the immersion-drawing phase inversion method, with PSF as the alkali-resistant polymer matrix and porous irregular ZrO2 nanoparticles as the hydrophilic additive. The experimental results showed that replacing commercial ZrO2 with porous irregular ZrO2 nanoparticles at an 85 wt% ZrO2 nanoparticle loading improved both bubble point pressure and current transmission efficiency, attributed to the change in the morphological structure of the ZrO2 nanoparticles. The P-Z85 composite separator membrane exhibited highly promising characteristics, with a high bubble point pressure of 3.76 bar and a low area resistance of 0.20 Ω cm2. Stability tests conducted in 30 wt% KOH electrolyte at 80 °C and a current density of 0.65 A cm−2 demonstrated excellent continuous electrolysis stability for the P-Z85 composite separator membrane. These results indicate that the PSF@ZrO2/PPS composite separator membrane prepared in this study exhibits excellent performance in 30 wt% KOH electrolyte, significantly extending its service life.

碱性水电解制氢是电解槽系统的关键组成部分,开发具有低面积电阻、高气泡点压力和长期安全稳定性的复合分离膜对于碱性水电解制氢至关重要。本研究以 PSF 为耐碱聚合物基体,以多孔不规则 ZrO2 纳米粒子为亲水添加剂,采用浸泡-拉伸反相法成功制备了 PPS 网布增强 PSF@ZrO2 复合分离膜。实验结果表明,在 ZrO2 纳米粒子含量为 85 wt%时,用多孔不规则 ZrO2 纳米粒子取代商用 ZrO2,可提高气泡点压力和电流传输效率,这归因于 ZrO2 纳米粒子形态结构的变化。P-Z85 复合分离膜表现出了很好的特性,气泡点压力高达 3.76 巴,面积电阻低至 0.20 Ω cm2。在温度为 80 °C 和电流密度为 0.65 A cm-2 的 30 wt% KOH 电解液中进行的稳定性测试表明,P-Z85 复合分离膜具有出色的连续电解稳定性。这些结果表明,本研究制备的 PSF@ZrO2/PPS 复合分离膜在 30 wt% KOH 电解液中表现出优异的性能,大大延长了其使用寿命。
{"title":"Effect of porous irregular ZrO2 nanoparticles on the performance of alkaline water electrolysis composite separator membranes under complex conditions","authors":"","doi":"10.1016/j.memsci.2024.123332","DOIUrl":"10.1016/j.memsci.2024.123332","url":null,"abstract":"<div><p>Developing composite separator membranes with low area resistance, high bubble point pressure, and long-term safety and stability is crucial for alkaline water electrolysis for hydrogen production as a key component of electrolyzer systems. In this study, PPS mesh fabric reinforced PSF@ZrO<sub>2</sub> composite separator membranes were successfully prepared using the immersion-drawing phase inversion method, with PSF as the alkali-resistant polymer matrix and porous irregular ZrO<sub>2</sub> nanoparticles as the hydrophilic additive. The experimental results showed that replacing commercial ZrO<sub>2</sub> with porous irregular ZrO<sub>2</sub> nanoparticles at an 85 wt% ZrO<sub>2</sub> nanoparticle loading improved both bubble point pressure and current transmission efficiency, attributed to the change in the morphological structure of the ZrO<sub>2</sub> nanoparticles. The P-Z85 composite separator membrane exhibited highly promising characteristics, with a high bubble point pressure of 3.76 bar and a low area resistance of 0.20 Ω cm<sup>2</sup>. Stability tests conducted in 30 wt% KOH electrolyte at 80 °C and a current density of 0.65 A cm<sup>−2</sup> demonstrated excellent continuous electrolysis stability for the P-Z85 composite separator membrane. These results indicate that the PSF@ZrO<sub>2</sub>/PPS composite separator membrane prepared in this study exhibits excellent performance in 30 wt% KOH electrolyte, significantly extending its service life.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142232113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Separation of xylene isomers controlled by adsorption configuration on fluorinated lamellar membrane 通过氟化片层膜上的吸附构型控制二甲苯异构体的分离
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-12 DOI: 10.1016/j.memsci.2024.123328

Separation of the xylene isomers has always been of great challenge and interest to the industry. Here, separation factors of 51 and 9 for p-/o-xylene and p-/m-xylene with a p-xylene permeance of 1.2 × 10−7 and 2.2 × 10−7 mol m−2 s−1 Pa−1, respectively, are achieved on the simple tandem fluorinated MXene lamellar membranes with 11%F and 1%F content through insight into the inversion behavior of the adsorption configuration enabled by the difference in dipole moments of xylenes under the combined interaction of xylene–CH3 F attraction and xylene–π–bond F repulsion. The favorable configuration of p-xylene maintains the flat adsorption, while that of m- and o-xylene undergoes a transition from upright to tilted and flat adsorption. DFT calculations confirm the weak flat adsorption of p-xylene on MXene-11%F repelled by the π–bond F repulsion and the strong upright adsorption of m- and o-xylene via the regulation of the repulsion, which contributes to a high throughput of p-xylene. As the F content decreases to 1 %, the low π–bond F repulsion results in strong flat configuration of p-xylene and weak flat configuration of m- and o-xylene. This work provides ideas for separating isomers by controlling the adsorption configuration through understanding their interaction forces in the membrane channel.

二甲苯异构体的分离一直是业界面临的巨大挑战和兴趣所在。在这里,对/邻二甲苯和对/间二甲苯的分离因子分别为 51 和 9,对二甲苯的渗透率分别为 1.2 × 10-7 和 2.在二甲苯-CH3 ... F吸引力和二甲苯-π键 ... F排斥力的共同作用下,二甲苯偶极矩的差异导致了吸附构型的反转行为。对二甲苯的有利构型保持了平吸附,而间二甲苯和邻二甲苯的有利构型则经历了从直立吸附到倾斜吸附和平吸附的转变。DFT 计算证实,对二甲苯在 MXene-11%F 上的π键......F 斥力作用下具有较弱的平吸附性,而间二甲苯和邻二甲苯则通过斥力调节具有较强的直立吸附性,这有助于提高对二甲苯的吞吐量。当 F 含量降至 1 % 时,低 π 键 ... F 斥力导致对二甲苯的强扁平构型和间二甲苯和邻二甲苯的弱扁平构型。这项研究通过了解膜通道中的相互作用力,为通过控制吸附构型来分离异构体提供了思路。
{"title":"Separation of xylene isomers controlled by adsorption configuration on fluorinated lamellar membrane","authors":"","doi":"10.1016/j.memsci.2024.123328","DOIUrl":"10.1016/j.memsci.2024.123328","url":null,"abstract":"<div><p>Separation of the xylene isomers has always been of great challenge and interest to the industry. Here, separation factors of 51 and 9 for <em>p</em>-/<em>o</em>-xylene and <em>p</em>-/<em>m</em>-xylene with a <em>p</em>-xylene permeance of 1.2 × 10<sup>−7</sup> and 2.2 × 10<sup>−7</sup> mol m<sup>−2</sup> s<sup>−1</sup> Pa<sup>−1</sup>, respectively, are achieved on the simple tandem fluorinated MXene lamellar membranes with 11%F and 1%F content through insight into the inversion behavior of the adsorption configuration enabled by the difference in dipole moments of xylenes under the combined interaction of xylene–CH<sub>3</sub> <sup>…</sup> F attraction and xylene–π–bond <sup>…</sup> F repulsion. The favorable configuration of <em>p</em>-xylene maintains the flat adsorption, while that of <em>m</em>- and <em>o</em>-xylene undergoes a transition from upright to tilted and flat adsorption. DFT calculations confirm the weak flat adsorption of <em>p</em>-xylene on MXene-11%F repelled by the π–bond <sup>…</sup> F repulsion and the strong upright adsorption of <em>m</em>- and <em>o</em>-xylene <em>via</em> the regulation of the repulsion, which contributes to a high throughput of <em>p</em>-xylene. As the F content decreases to 1 %, the low π–bond <sup>…</sup> F repulsion results in strong flat configuration of <em>p</em>-xylene and weak flat configuration of <em>m</em>- and <em>o</em>-xylene. This work provides ideas for separating isomers by controlling the adsorption configuration through understanding their interaction forces in the membrane channel.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142229211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bifunctionalized MOFs modified poly (aryl ether ketone sulfone) ultrafiltration membranes with high-efficient BSA separation and dye adsorption 具有高效 BSA 分离和染料吸附功能的双官能化 MOFs 改性聚(芳基醚酮砜)超滤膜
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-12 DOI: 10.1016/j.memsci.2024.123318

In this study, by connecting the amino ligand in ZIF-8-NH2 with an alkyl side chain containing sulfonic acid groups in a one-step method, a novel nanofiller (ZIF-8-NS) with bifunctional amino and sulfonic acid groups was formed. Sulfonated poly (aryl ether ketone sulfone) containing fluorene group (F-SPAEKS) was chosen as the polymer matrix. The nanofiller not only had good hydrophilicity but also had electrostatic interaction with the polymer matrix, which effectively promoted the compatibility problem among the polymer matrix and the filler. The nanofillers were characterized by XRD, FT-IR, SEM and XPS. The composite membranes were prepared by the NIPs method. The antifouling and separation properties of the prepared mixed matrix membranes (MMMs) were investigated using positively charged dye (RHB) and negative charge bovine serum albumin (BSA) as model contaminants. The water flux of the pure membrane achieved 529.16 L/m2 h. When the addition amount of ZIF-8-NS was 0.1 %, the water flux of M4 (F-SPAEKS/ZIF-8-NS-0.1 %) could reach 838.84 L/m2 h. The retention rate of the BSA solution could reach 99.06 %, and the FRR value was kept at a high level (81.45 %). Meanwhile, the dynamic retention of M4 on the primary adsorption of the dye RHB could even reach 99.89 %. Therefore, the innovative design of the novel MMMs not only improved the flux, retention, and other separation properties but also enhanced their excellent adsorption capacity for RHB dyes. This result indicated that the nanofiller ZIF-8-NS provided an interesting reference for the study of ultrafiltration membranes.

本研究采用一步法将 ZIF-8-NH2 中的氨基配体与含有磺酸基团的烷基侧链连接起来,形成了一种具有双功能氨基和磺酸基团的新型纳米填料(ZIF-8-NS)。聚合物基质选用了含芴基团的磺化聚(芳基醚酮砜)(F-SPAEKS)。该纳米填料不仅具有良好的亲水性,而且与聚合物基体具有静电作用,从而有效地解决了聚合物基体与填料之间的相容性问题。对纳米填料进行了 XRD、FT-IR、SEM 和 XPS 表征。采用 NIPs 法制备了复合膜。以带正电荷的染料(RHB)和带负电荷的牛血清白蛋白(BSA)为模型污染物,研究了制备的混合基质膜(MMMs)的防污和分离性能。当 ZIF-8-NS 的添加量为 0.1 % 时,M4(F-SPAEKS/ZIF-8-NS-0.1 %)的水通量达到 838.84 L/m2 h,BSA 溶液的截留率达到 99.06 %,FRR 值保持在较高水平(81.45 %)。同时,M4 对染料 RHB 一次吸附的动态截留率甚至达到了 99.89 %。因此,新型 MMM 的创新设计不仅提高了通量、截留率和其他分离性能,还增强了其对 RHB 染料的出色吸附能力。这一结果表明,纳米填料 ZIF-8-NS 为超滤膜的研究提供了有趣的参考。
{"title":"Bifunctionalized MOFs modified poly (aryl ether ketone sulfone) ultrafiltration membranes with high-efficient BSA separation and dye adsorption","authors":"","doi":"10.1016/j.memsci.2024.123318","DOIUrl":"10.1016/j.memsci.2024.123318","url":null,"abstract":"<div><p>In this study, by connecting the amino ligand in ZIF-8-NH<sub>2</sub> with an alkyl side chain containing sulfonic acid groups in a one-step method, a novel nanofiller (ZIF-8-NS) with bifunctional amino and sulfonic acid groups was formed. Sulfonated poly (aryl ether ketone sulfone) containing fluorene group (F-SPAEKS) was chosen as the polymer matrix. The nanofiller not only had good hydrophilicity but also had electrostatic interaction with the polymer matrix, which effectively promoted the compatibility problem among the polymer matrix and the filler. The nanofillers were characterized by XRD, FT-IR, SEM and XPS. The composite membranes were prepared by the NIPs method. The antifouling and separation properties of the prepared mixed matrix membranes (MMMs) were investigated using positively charged dye (RHB) and negative charge bovine serum albumin (BSA) as model contaminants. The water flux of the pure membrane achieved 529.16 L/m<sup>2</sup> h. When the addition amount of ZIF-8-NS was 0.1 %, the water flux of M4 (F-SPAEKS/ZIF-8-NS-0.1 %) could reach 838.84 L/m<sup>2</sup> h. The retention rate of the BSA solution could reach 99.06 %, and the FRR value was kept at a high level (81.45 %). Meanwhile, the dynamic retention of M4 on the primary adsorption of the dye RHB could even reach 99.89 %. Therefore, the innovative design of the novel MMMs not only improved the flux, retention, and other separation properties but also enhanced their excellent adsorption capacity for RHB dyes. This result indicated that the nanofiller ZIF-8-NS provided an interesting reference for the study of ultrafiltration membranes.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142173420","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mixed matrix membrane-based transport membrane condenser for improving the waste heat recovery performance in carbon capture process 基于混合基质膜的传输膜冷凝器,用于提高碳捕集过程中的余热回收性能
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-12 DOI: 10.1016/j.memsci.2024.123325

Applying a transport membrane condenser (TMC) based on the hydrophilic ceramic membrane to recover the waste heat from the hot stripped gas could effectively reduce the heat consumption of CO2 regeneration in the carbon capture process. However, the high cost of ceramic membrane hindered the development of this technology. So in this study, a novel mixed matrix membrane (MMM) was proposed to replace the conventional ceramic membrane. MMMs were prepared by mixing carbon nanotube (CNT) into polyvinylidene fluoride (PVDF) casting solution through non-solvent phase separation method, and then were adopted for the waste heat recovery from the stripped gas featured with the molar ratio of CO2 to H2O(g) of 1:1∼1:2. Furthermore, the heat transfer resistance between the stripped gas and bypassed CO2-rich solvent when adopting MMMs was also analyzed through computational fluid dynamics (CFD). Results indicated that the addition of CNT or hydroxylated CNT (CNT-OH) effectively enhanced the heat recovery performance of MMMs. Moreover, MMMs prepared by mixing CNT-OH and hydroxylated boron nitride (BN–OH) further boosted the heat flux, achieving a maximum value of 23.72 MJ/(m2·h), representing an increase of up to 8.41 % compared to the original PVDF membrane without adding any additives. At the experimental conditions in this study, the gas-side individual thermal resistance dominated the overall thermal resistance and consequently the heat transfer performance. With an increase in the stripped gas flow rate, the ratio of individual heat transfer resistance of membrane to the overall resistance increased. Notably, the installation of baffles on the gas side of TMC reduced the gas-side thermal resistance. In this study, the optimum thermal conductivity of the organic membrane increased with the waste heat recovery scale from stripped gas. In addition, when the thermal conductivity of membrane exceeded 4 W/(m·°C), the increase in thermal conductivity on the waste heat recovery was not significant. This study confirmed the application potential of MMMs in the waste heat recovery.

应用基于亲水陶瓷膜的传输膜冷凝器(TMC)回收热剥离气体中的余热,可有效降低碳捕集过程中二氧化碳再生的热量消耗。然而,陶瓷膜的高成本阻碍了这一技术的发展。因此,本研究提出了一种新型混合基质膜(MMM)来替代传统的陶瓷膜。通过非溶剂相分离法将碳纳米管(CNT)混合到聚偏氟乙烯(PVDF)浇铸溶液中制备出混合基质膜,然后采用混合基质膜从 CO2 与 H2O(g)的摩尔比为 1:1∼1:2 的剥离气体中回收余热。此外,还通过计算流体动力学(CFD)分析了采用 MMMs 时剥离气体与旁路富二氧化碳溶剂之间的传热阻力。结果表明,添加 CNT 或羟基 CNT(CNT-OH)可有效提高 MMMs 的热回收性能。此外,CNT-OH 和羟基氮化硼(BN-OH)混合制备的 MMM 进一步提高了热通量,最大值达到 23.72 MJ/(m2-h),与未添加任何添加剂的原始 PVDF 膜相比,提高了 8.41%。在本研究的实验条件下,气体侧的单个热阻主导了整体热阻,从而影响了传热性能。随着剥离气体流速的增加,膜的单个热传导阻力与整体阻力之比增加。值得注意的是,在 TMC 气体侧安装挡板降低了气体侧热阻。在这项研究中,有机膜的最佳导热率随着剥离气体余热回收规模的扩大而增加。此外,当膜的热导率超过 4 W/(m-°C) 时,热导率对废热回收的影响并不显著。这项研究证实了 MMM 在余热回收中的应用潜力。
{"title":"Mixed matrix membrane-based transport membrane condenser for improving the waste heat recovery performance in carbon capture process","authors":"","doi":"10.1016/j.memsci.2024.123325","DOIUrl":"10.1016/j.memsci.2024.123325","url":null,"abstract":"<div><p>Applying a transport membrane condenser (TMC) based on the hydrophilic ceramic membrane to recover the waste heat from the hot stripped gas could effectively reduce the heat consumption of CO<sub>2</sub> regeneration in the carbon capture process. However, the high cost of ceramic membrane hindered the development of this technology. So in this study, a novel mixed matrix membrane (MMM) was proposed to replace the conventional ceramic membrane. MMMs were prepared by mixing carbon nanotube (CNT) into polyvinylidene fluoride (PVDF) casting solution through non-solvent phase separation method, and then were adopted for the waste heat recovery from the stripped gas featured with the molar ratio of CO<sub>2</sub> to H<sub>2</sub>O(g) of 1:1∼1:2. Furthermore, the heat transfer resistance between the stripped gas and bypassed CO<sub>2</sub>-rich solvent when adopting MMMs was also analyzed through computational fluid dynamics (CFD). Results indicated that the addition of CNT or hydroxylated CNT (CNT-OH) effectively enhanced the heat recovery performance of MMMs. Moreover, MMMs prepared by mixing CNT-OH and hydroxylated boron nitride (BN–OH) further boosted the heat flux, achieving a maximum value of 23.72 MJ/(m<sup>2</sup>·h), representing an increase of up to 8.41 % compared to the original PVDF membrane without adding any additives. At the experimental conditions in this study, the gas-side individual thermal resistance dominated the overall thermal resistance and consequently the heat transfer performance. With an increase in the stripped gas flow rate, the ratio of individual heat transfer resistance of membrane to the overall resistance increased. Notably, the installation of baffles on the gas side of TMC reduced the gas-side thermal resistance. In this study, the optimum thermal conductivity of the organic membrane increased with the waste heat recovery scale from stripped gas. In addition, when the thermal conductivity of membrane exceeded 4 W/(m·°C), the increase in thermal conductivity on the waste heat recovery was not significant. This study confirmed the application potential of MMMs in the waste heat recovery.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142229937","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Real-time AFM analysis of the impact of CO2 on solid-supported ionic liquid nanomembranes 二氧化碳对固体支撑离子液体纳米膜影响的实时原子力显微镜分析
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-12 DOI: 10.1016/j.memsci.2024.123330

Ionic liquids (ILs) have excellent ability to capture CO2 due to their unique properties. The observation on the evolution process of solid-supported IL nanomembranes at the nanoscale benefits understanding the interaction between IL nanomembranes and CO2. In this work, we have investigated the CO2-induced evolution process of solid-supported nanomembranes formed by the imidazolium-based ILs with alkyl chains of different lengths but with a common anion by in-situ atomic force microscopy (AFM). The morphology evolution and mechanical properties of the IL nanomembranes have been quantitatively analyzed. The results show that similar phenomena were observed for the three IL nanomembranes, i.e., the absorption of CO2 presents a maximal impact on the innermost layer of the solid-supported IL nanomembranes. The innermost layer of IL nanomembranes becomes fragmented and tends to re-assemble into a multi-layer structure, while the area of the multi-layer IL nanomembranes expands due to the incorporation of some small regions. In addition, the morphology changes of IL nanomembranes are dependent on the length of cation alkyl side chain. For the [BMI][TFSI] nanomembrane, the morphology change is faster than the other two IL nanomembranes in the preliminary stage of CO2 absorption and reaches a stable state in a shorter time. AFM quantitative nanomechanical measurements show that Young's moduli of the three IL nanomembranes significantly decrease after CO2 absorption, which supports that CO2 molecules could weaken the interaction among IL anions, cations and mica, and thus lead to the morphology changes of the three solid-supported IL nanomembranes. Our work provides microscopic insights into the process of CO2 absorption by ILs, which lays a foundation for further studying the interaction between CO2 and solid-supported IL nanomembranes.

离子液体(IL)因其独特的性质而具有捕获二氧化碳的卓越能力。在纳米尺度上观察固体支撑的离子液体纳米膜的演化过程有助于理解离子液体纳米膜与二氧化碳之间的相互作用。在这项工作中,我们通过原位原子力显微镜(AFM)研究了由烷基链长度不同但具有共同阴离子的咪唑基IL形成的固体支撑纳米膜的二氧化碳诱导演化过程。定量分析了IL纳米膜的形态演变和机械性能。结果表明,三种 IL 纳米膜都出现了类似的现象,即二氧化碳的吸收对固体支撑的 IL 纳米膜最内层的影响最大。IL 纳米膜的最内层变得支离破碎,并趋向于重新组装成多层结构,而多层 IL 纳米膜的面积则由于一些小区域的加入而扩大。此外,IL 纳米膜的形态变化与阳离子烷基侧链的长度有关。对于[BMI][TFSI]纳米膜来说,在吸收二氧化碳的初级阶段,其形态变化比其他两种IL纳米膜更快,并在更短的时间内达到稳定状态。原子力显微镜(AFM)纳米力学定量测量表明,三种IL纳米膜的杨氏模量在吸收二氧化碳后显著下降,这证明二氧化碳分子可以削弱IL阴、阳离子和云母之间的相互作用,从而导致三种固体支撑的IL纳米膜的形貌发生变化。我们的研究从微观上揭示了IL吸收二氧化碳的过程,为进一步研究二氧化碳与固体支撑的IL纳米膜之间的相互作用奠定了基础。
{"title":"Real-time AFM analysis of the impact of CO2 on solid-supported ionic liquid nanomembranes","authors":"","doi":"10.1016/j.memsci.2024.123330","DOIUrl":"10.1016/j.memsci.2024.123330","url":null,"abstract":"<div><p>Ionic liquids (ILs) have excellent ability to capture CO<sub>2</sub> due to their unique properties. The observation on the evolution process of solid-supported <span>IL</span> nanomembranes at the nanoscale benefits understanding the interaction between <span>IL</span> nanomembranes and CO<sub>2</sub>. In this work, we have investigated the CO<sub>2</sub>-induced evolution process of solid-supported nanomembranes formed by the imidazolium-based ILs with alkyl chains of different lengths but with a common anion by in-situ atomic force microscopy (AFM). The morphology evolution and mechanical properties of the IL nanomembranes have been quantitatively analyzed. The results show that similar phenomena were observed for the three <span>IL</span> nanomembranes, i.e., the absorption of CO<sub>2</sub> presents a maximal impact on the innermost layer of the solid-supported <span>IL</span> nanomembranes. The innermost layer of IL nanomembranes becomes fragmented and tends to re-assemble into a multi-layer structure, while the area of the multi-layer IL nanomembranes expands due to the incorporation of some small regions. In addition, the morphology changes of IL nanomembranes are dependent on the length of cation alkyl side chain. For the [BMI][TFSI] nanomembrane, the morphology change is faster than the other two IL nanomembranes in the preliminary stage of CO<sub>2</sub> absorption and reaches a stable state in a shorter time. <span>AFM</span> quantitative nanomechanical measurements show that Young's moduli of the three <span>IL</span> nanomembranes significantly decrease after CO<sub>2</sub> absorption, which supports that CO<sub>2</sub> molecules could weaken the interaction among <span>IL</span> anions, cations and mica, and thus lead to the morphology changes of the three solid-supported <span>IL</span> nanomembranes. Our work provides microscopic insights into the process of CO<sub>2</sub> absorption by ILs, which lays a foundation for further studying the interaction between CO<sub>2</sub> and solid-supported <span>IL</span> nanomembranes.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142233602","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sulfonated polybenzimidazole membrane with graphene oxide additive for 2,3-butanediol/water separation: A molecular simulation 含氧化石墨烯添加剂的磺化聚苯并咪唑膜用于 2,3 丁二醇/水分离:分子模拟
IF 8.4 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2024-09-12 DOI: 10.1016/j.memsci.2024.123312

Membrane separation for 2,3-butanediol (2,3-BDO) recovery from fermentation broth is highly valued for sustainable and renewable processes, but it requires efficient membrane materials. This work evaluates the sulfonated polybenzimidazole (sPBI) and its graphene oxide (GO) doped composite membrane for separating 2,3-BDO and water via atomistic simulations. Density functional theory calculations are applied to identify various forms of sPBI structures and quantify their binding interactions with 2,3-BDO and water. Classical molecular dynamic simulations are used to evaluate the structural changes, diffusivity, and selectivity of 2,3-BDO and water in different sPBI models, GO surfaces, and GO-doped sPBI composite models. Our results suggest that sPBI slightly increases the crystallinity of the membrane structures, enhances the adsorption strength for both 2,3-BDO and water, and improves the water/2,3-BDO selectivity by 2–3 times. The GO surfaces display a maximum selectivity at a surface coverage of 0.1–0.15 for both hydroxyl and epoxy surface groups. The addition of GO flakes to sPBI creates new interaction sites for 2,3-BDO and water at the interface of sPBI and GO, and the water/2,3-BDO selectivity of GO-doped sPBI models is further increased up to 3 times. This work illustrates how the integrated addition of sPBI and GO flakes offers a promising approach to selective separation of 2,3-BDO and water, providing theoretical guidance for polybenzimidazole-based membranes in the potential application of 2,3-BDO recovery.

从发酵液中回收 2,3-丁二醇(2,3-BDO)的膜分离在可持续和可再生工艺中具有很高的价值,但这需要高效的膜材料。本研究通过原子模拟评估了磺化聚苯并咪唑(sPBI)及其掺杂氧化石墨烯(GO)的复合膜在分离 2,3-BDO 和水方面的应用。应用密度泛函理论计算确定了各种形式的 sPBI 结构,并量化了它们与 2,3-BDO 和水的结合相互作用。经典分子动力学模拟用于评估 2,3-BDO 和水在不同 sPBI 模型、GO 表面和掺杂 GO 的 sPBI 复合模型中的结构变化、扩散性和选择性。我们的研究结果表明,sPBI 稍微增加了膜结构的结晶度,增强了对 2,3-BDO 和水的吸附强度,并将水/2,3-BDO 的选择性提高了 2-3 倍。在羟基和环氧表面基团的表面覆盖率为 0.1-0.15 时,GO 表面的选择性最大。在 sPBI 和 GO 的界面上添加片状 GO 可为 2,3-BDO 和水创造新的相互作用位点,掺杂 GO 的 sPBI 模型的水/2,3-BDO 选择性可进一步提高 3 倍。这项工作说明了综合添加 sPBI 和 GO 片如何为 2,3-BDO 和水的选择性分离提供了一种前景广阔的方法,为聚苯并咪唑基膜在 2,3-BDO 回收的潜在应用中提供了理论指导。
{"title":"Sulfonated polybenzimidazole membrane with graphene oxide additive for 2,3-butanediol/water separation: A molecular simulation","authors":"","doi":"10.1016/j.memsci.2024.123312","DOIUrl":"10.1016/j.memsci.2024.123312","url":null,"abstract":"<div><p>Membrane separation for 2,3-butanediol (2,3-BDO) recovery from fermentation broth is highly valued for sustainable and renewable processes, but it requires efficient membrane materials. This work evaluates the sulfonated polybenzimidazole (sPBI) and its graphene oxide (GO) doped composite membrane for separating 2,3-BDO and water via atomistic simulations. Density functional theory calculations are applied to identify various forms of sPBI structures and quantify their binding interactions with 2,3-BDO and water. Classical molecular dynamic simulations are used to evaluate the structural changes, diffusivity, and selectivity of 2,3-BDO and water in different sPBI models, GO surfaces, and GO-doped sPBI composite models. Our results suggest that sPBI slightly increases the crystallinity of the membrane structures, enhances the adsorption strength for both 2,3-BDO and water, and improves the water/2,3-BDO selectivity by 2–3 times. The GO surfaces display a maximum selectivity at a surface coverage of 0.1–0.15 for both hydroxyl and epoxy surface groups. The addition of GO flakes to sPBI creates new interaction sites for 2,3-BDO and water at the interface of sPBI and GO, and the water/2,3-BDO selectivity of GO-doped sPBI models is further increased up to 3 times. This work illustrates how the integrated addition of sPBI and GO flakes offers a promising approach to selective separation of 2,3-BDO and water, providing theoretical guidance for polybenzimidazole-based membranes in the potential application of 2,3-BDO recovery.</p></div>","PeriodicalId":368,"journal":{"name":"Journal of Membrane Science","volume":null,"pages":null},"PeriodicalIF":8.4,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142240457","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
Journal of Membrane Science
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1