An innovative strategy was proposed by integration of membrane contactor (MC) with biphasic solvent for efficient CO capture from flue gas. The accessible fly ash-based ceramic membrane (CM) underwent hydrophobic modification through silane grafting, followed by fluoroalkylsilane decoration, to prepare the superhydrophobic membrane (CSCM). The CSCM significantly improved resistance to wetting by the biphasic solvent, consisting of amine (DETA) and sulfolane (TMS). Morphological characterizations and chemical analysis revealed the notable enhancements in pore structure and hydrophobic chemical groups for the modified membrane. Predictions of wetting/bubbling behavior based on static wetting theory referred the liquid entry pressure (LEP) of CSCM increased by 20 kPa compared to pristine CM. Compared with traditional amine solvents, the biphasic solvent presented the expected phase separation. Performance experiments demonstrated that the CO capture efficiency of the biphasic solvent increased by 7%, and the electrical energy required for desorption decreased by 32%. The 60-h continuous testing and supplemental characterization of used membrane confirmed the excellent adaptability and durability of the CSCMs. This study provides a potential approach for accessing hydrophobic ceramic membranes and biphasic solvents for industrial CO capture.
通过将膜接触器（MC）与双相溶剂相结合，提出了一种从烟道气中高效捕集一氧化碳的创新策略。通过硅烷接枝对可获得的粉煤灰基陶瓷膜（CM）进行疏水改性，然后进行氟烷基硅烷装饰，制备出超疏水膜（CSCM）。CSCM 大大提高了抗双相溶剂（由胺（DETA）和砜（TMS）组成）润湿的能力。形态特征和化学分析显示，改性膜的孔隙结构和疏水化学基团明显改善。基于静态润湿理论的润湿/气泡行为预测表明，与原始 CM 相比，CSCM 的液体进入压力 (LEP) 增加了 20 kPa。与传统胺溶剂相比，双相溶剂呈现出预期的相分离现象。性能实验表明，双相溶剂的一氧化碳捕获效率提高了 7%，解吸所需的电能降低了 32%。对使用过的膜进行的 60 小时连续测试和补充表征证实了 CSCM 的出色适应性和耐用性。这项研究为利用疏水陶瓷膜和双相溶剂捕获工业 CO 提供了一种潜在的方法。
{"title":"Superhydrophobic ceramic membrane coupled with a biphasic solvent for efficient CO2 capture","authors":"Kaili Xue, Zhen Chen, Xiaona Wu, Heng Zhang, Haiping Chen, Junhua Li","doi":"10.1016/j.gee.2024.07.010","DOIUrl":"https://doi.org/10.1016/j.gee.2024.07.010","url":null,"abstract":"An innovative strategy was proposed by integration of membrane contactor (MC) with biphasic solvent for efficient CO capture from flue gas. The accessible fly ash-based ceramic membrane (CM) underwent hydrophobic modification through silane grafting, followed by fluoroalkylsilane decoration, to prepare the superhydrophobic membrane (CSCM). The CSCM significantly improved resistance to wetting by the biphasic solvent, consisting of amine (DETA) and sulfolane (TMS). Morphological characterizations and chemical analysis revealed the notable enhancements in pore structure and hydrophobic chemical groups for the modified membrane. Predictions of wetting/bubbling behavior based on static wetting theory referred the liquid entry pressure (LEP) of CSCM increased by 20 kPa compared to pristine CM. Compared with traditional amine solvents, the biphasic solvent presented the expected phase separation. Performance experiments demonstrated that the CO capture efficiency of the biphasic solvent increased by 7%, and the electrical energy required for desorption decreased by 32%. The 60-h continuous testing and supplemental characterization of used membrane confirmed the excellent adaptability and durability of the CSCMs. This study provides a potential approach for accessing hydrophobic ceramic membranes and biphasic solvents for industrial CO capture.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"23 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141935020","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}
A two-stage catalytic membrane reactor (CMR) that couples CO splitting with methane oxidation reactions was constructed based on an oxygen-permeable perovskite asymmetric membrane. The asymmetric membrane comprises a dense SrFeTaO (SFT) separation layer and a porous Sr(FeTa)CuO (SFTC) catalytic layer. In the first stage reactor, a CO splitting reaction (CDS: 2CO→2CO+O) occurs at the SFTC catalytic layer. Subsequently, the O product is selectively extracted through the SFT separation layer to the permeated side for the methane combustion reaction (MCR), which provides an extremely low oxygen partial pressure to enhance the oxygen extraction. In the second stage, a Sr(FeTa)NiO (SFTN) catalyst is employed to reform the products derived from MCR. The two-stage CMR design results in a remarkable 35.4% CO conversion for CDS at 900 °C. The two-stage CMR was extended to a hollow fiber configuration combining with solar irradiation. The solar-assisted two-stage CMR can operate stably for over 50 hours with a high hydrogen yield of 18.1 mL min cm. These results provide a novel strategy for reducing CO emissions, suggesting potential avenues for the design of the high-performance CMRs and catalysts based on perovskite oxides in the future.
基于透氧包晶石非对称膜，构建了一种两级催化膜反应器（CMR），可将一氧化碳分离与甲烷氧化反应结合起来。不对称膜由致密的 SrFeTaO（SFT）分离层和多孔的 Sr（FeTa）CuO（SFTC）催化层组成。在第一级反应器中，SFTC 催化层发生 CO 分离反应（CDS：2CO→2CO+O）。随后，O 产物通过 SFT 分离层被选择性地萃取到渗透侧，进行甲烷燃烧反应（MCR），该反应提供了极低的氧分压，以提高氧气萃取率。在第二阶段，采用 Sr(FeTa)NiO (SFTN) 催化剂对 MCR 产生的产物进行重整。两段式 CMR 设计使 CDS 在 900 °C 下的 CO 转化率达到 35.4%。两级 CMR 扩展到中空纤维配置，并与太阳能照射相结合。太阳能辅助的双级 CMR 可稳定运行 50 小时以上，氢气产量高达 18.1 mL min cm。这些结果为减少一氧化碳排放提供了一种新的策略，为将来设计基于过氧化物氧化物的高性能 CMR 和催化剂提供了潜在的途径。
{"title":"Solar-assisted two-stage catalytic membrane reactor for coupling CO2 splitting with methane oxidation reaction","authors":"Jinkun Tan, Zhenbin Gu, Zhengkun Liu, Pei Wang, Reinout Meijboom, Guangru Zhang, Wanqin Jin","doi":"10.1016/j.gee.2024.07.006","DOIUrl":"https://doi.org/10.1016/j.gee.2024.07.006","url":null,"abstract":"A two-stage catalytic membrane reactor (CMR) that couples CO splitting with methane oxidation reactions was constructed based on an oxygen-permeable perovskite asymmetric membrane. The asymmetric membrane comprises a dense SrFeTaO (SFT) separation layer and a porous Sr(FeTa)CuO (SFTC) catalytic layer. In the first stage reactor, a CO splitting reaction (CDS: 2CO→2CO+O) occurs at the SFTC catalytic layer. Subsequently, the O product is selectively extracted through the SFT separation layer to the permeated side for the methane combustion reaction (MCR), which provides an extremely low oxygen partial pressure to enhance the oxygen extraction. In the second stage, a Sr(FeTa)NiO (SFTN) catalyst is employed to reform the products derived from MCR. The two-stage CMR design results in a remarkable 35.4% CO conversion for CDS at 900 °C. The two-stage CMR was extended to a hollow fiber configuration combining with solar irradiation. The solar-assisted two-stage CMR can operate stably for over 50 hours with a high hydrogen yield of 18.1 mL min cm. These results provide a novel strategy for reducing CO emissions, suggesting potential avenues for the design of the high-performance CMRs and catalysts based on perovskite oxides in the future.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"134 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141779681","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}
Electrochemical reduction of CO is a promising approach to convert CO to high-valued chemicals and fuels. However, developing efficient electrocatalysts featuring desirable activity and selectivity is still a big challenge. In this work, a strategy of introducing functionalized molecules with desirable CO affinity to regulate Ag catalyst for promoting electrochemical reduction of CO was proposed. Specifically, 3-mercapto-1,2,4-triazole was introduced onto the Ag nanoparticle (Ag-m-Triz) for the first time to achieve selectively converting CO to carbon monoxide (CO). This Ag-m-Triz exhibits excellent performance for CO reduction with a high CO Faradaic efficiency (FE) of 99.2% and CO partial current density of 85.0 mA cm at −2.3 V vs. Ag/Ag in H-cell when combined with the ionic liquid-based electrolyte, 30 wt% 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim][PF])-65 wt% acetonitrile (AcN)-5 wt% HO, which is 2.5-fold higher than the current density in Ag-powder under the same condition. Mechanism studies confirm that the significantly improved performance of Ag-m-Triz originates from (i) the stronger adsorption ability of CO molecule and (ii) the weaker binding energy to form the COOH∗ intermediate on the surface of Ag-m-Triz compared with the Ag-powder catalyst, which boosts the conversion of CO to CO. This research provides a facile way to regulate electrocatalysts for efficient CO reduction by introducing functionalized molecules.
一氧化碳的电化学还原是将一氧化碳转化为高价值化学品和燃料的一种前景广阔的方法。然而，开发具有理想活性和选择性的高效电催化剂仍是一项巨大挑战。在这项工作中，我们提出了一种将具有理想 CO 亲和性的官能化分子引入银催化剂的策略，以促进 CO 的电化学还原。具体而言，首次在银纳米粒子（Ag-m-Triz）上引入了 3-巯基-1,2,4-三唑，以实现将一氧化碳（CO）选择性地转化为一氧化碳（CO）。这种 Ag-m-Triz 在一氧化碳还原方面表现出色，一氧化碳法拉第效率 (FE) 高达 99.2%，一氧化碳部分电流密度为 85.0 mA cm，电压为 -2.3 V。当与离子液体型电解质（30 wt% 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim][PF])-65 wt% acetonitrile (AcN)-5 wt% HO）结合使用时，在 H-cell 中的 Ag/Ag 部分电流密度为 85.0 mA cm，比相同条件下 Ag 粉末的电流密度高 2.5 倍。机理研究证实，Ag-m-Triz 性能的显著提高源于：(i) 与 Ag 粉末催化剂相比，Ag-m-Triz 对 CO 分子的吸附能力更强；(ii) 在 Ag-m-Triz 表面形成 COOH∗ 中间体的结合能更弱，从而促进了 CO 向 CO 的转化。这项研究提供了一种简便的方法，通过引入功能化分子来调节电催化剂，从而实现高效的 CO 还原。
{"title":"Boosting electrochemical reduction of CO2 to CO using molecule-regulated Ag nanoparticle in ionic liquids","authors":"Fangfang Li, Kuilin Peng, Chongyang Jiang, Shaojuan Zeng, Xiangping Zhang, Xiaoyan Ji","doi":"10.1016/j.gee.2024.07.005","DOIUrl":"https://doi.org/10.1016/j.gee.2024.07.005","url":null,"abstract":"Electrochemical reduction of CO is a promising approach to convert CO to high-valued chemicals and fuels. However, developing efficient electrocatalysts featuring desirable activity and selectivity is still a big challenge. In this work, a strategy of introducing functionalized molecules with desirable CO affinity to regulate Ag catalyst for promoting electrochemical reduction of CO was proposed. Specifically, 3-mercapto-1,2,4-triazole was introduced onto the Ag nanoparticle (Ag-m-Triz) for the first time to achieve selectively converting CO to carbon monoxide (CO). This Ag-m-Triz exhibits excellent performance for CO reduction with a high CO Faradaic efficiency (FE) of 99.2% and CO partial current density of 85.0 mA cm at −2.3 V vs. Ag/Ag in H-cell when combined with the ionic liquid-based electrolyte, 30 wt% 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim][PF])-65 wt% acetonitrile (AcN)-5 wt% HO, which is 2.5-fold higher than the current density in Ag-powder under the same condition. Mechanism studies confirm that the significantly improved performance of Ag-m-Triz originates from (i) the stronger adsorption ability of CO molecule and (ii) the weaker binding energy to form the COOH∗ intermediate on the surface of Ag-m-Triz compared with the Ag-powder catalyst, which boosts the conversion of CO to CO. This research provides a facile way to regulate electrocatalysts for efficient CO reduction by introducing functionalized molecules.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"414 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141779730","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}
Pub Date : 2024-07-05DOI: 10.1016/j.gee.2024.07.002
Yanghe Fu, Yijing Gao, Huilin Jia, Yuncai Zhao, Yan Feng, Weidong Zhu, Fumin Zhang, Morris D. Argyle, Maohong Fan
Three large π-conjugated and imine-based COFs, named TFP-TAB, TFP-TTA, and TTA-TTB, were synthesized via the ordered incorporation of benzene and triazine rings in the same host framework to study how the structural units affect the efficiency of CO photoreduction. Results from both experiments and density-functional theory (DFT) calculations indicate the separation and transfer of the photoinduced charges is highly related to the triazine-N content and the conjugation degree in the skeletons of COFs. High-efficiency CO photoreduction can be achieved by rationally adjusting the number and position of both benzene and triazine rings in the COFs. Specifically, TTA-TTB, with orderly interlaced triazine-benzene heterojunctions, can suppress the recombination probability of electrons and holes, which effectively immobilizes the key species (COOH) and lowers the free energy change of the potential-determining step, and thus exhibits a superior visible-light-induced photocatalytic activity that yields 121.7 μmol HCOOH g h. This research, therefore, helps to elucidate the effects of the different structural blocks in COFs on inherent heterogeneous photocatalysis for CO reduction at a molecular level.
为了研究结构单元如何影响 CO 的光诱导效率，我们通过在同一宿主框架中有序地加入苯环和三嗪环的方法合成了三种大的π共轭和亚胺基 COF，分别命名为 TFP-TAB、TFP-TTA 和 TTA-TTB。实验和密度泛函理论（DFT）计算的结果表明，光诱导电荷的分离和转移与 COFs 骨架中三嗪-N 的含量和共轭度密切相关。通过合理调整 COF 中苯环和三嗪环的数量和位置，可以实现高效的 CO 光还原。具体来说，TTA-TTB 具有有序交错的三嗪-苯异质结，可以抑制电子和空穴的重组概率，从而有效地固定了关键物种（COOH），降低了电位决定步骤的自由能变化，因此表现出卓越的可见光诱导光催化活性，可产生 121.7 μmol HCOOH g h。因此，这项研究有助于从分子层面阐明 COFs 中不同结构单元对固有异相光催化还原 CO 的影响。
{"title":"Rational engineering of triazine-benzene linked covalent-organic frameworks for efficient CO2 photoreduction","authors":"Yanghe Fu, Yijing Gao, Huilin Jia, Yuncai Zhao, Yan Feng, Weidong Zhu, Fumin Zhang, Morris D. Argyle, Maohong Fan","doi":"10.1016/j.gee.2024.07.002","DOIUrl":"https://doi.org/10.1016/j.gee.2024.07.002","url":null,"abstract":"Three large π-conjugated and imine-based COFs, named TFP-TAB, TFP-TTA, and TTA-TTB, were synthesized via the ordered incorporation of benzene and triazine rings in the same host framework to study how the structural units affect the efficiency of CO photoreduction. Results from both experiments and density-functional theory (DFT) calculations indicate the separation and transfer of the photoinduced charges is highly related to the triazine-N content and the conjugation degree in the skeletons of COFs. High-efficiency CO photoreduction can be achieved by rationally adjusting the number and position of both benzene and triazine rings in the COFs. Specifically, TTA-TTB, with orderly interlaced triazine-benzene heterojunctions, can suppress the recombination probability of electrons and holes, which effectively immobilizes the key species (COOH) and lowers the free energy change of the potential-determining step, and thus exhibits a superior visible-light-induced photocatalytic activity that yields 121.7 μmol HCOOH g h. This research, therefore, helps to elucidate the effects of the different structural blocks in COFs on inherent heterogeneous photocatalysis for CO reduction at a molecular level.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"78 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141586145","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}
LiPSCl is a highly wanted sulfide-solid-electrolyte (SSE) for developing all-solid-state lithium batteries, due to its high ionic conductivity, good processability and abundant compositional elements. However, its cyclability is poor because of harmful side reactions at the LiPSCl/Li interface and growth of lithium dendrites inside LiPSCl phase. Herein, we report a simple interface-engineering remedy to boost the electrochemical performance of LiPSCl, by coating its surface with a Li-compatible electrolyte LiOCl having low electronic conductivity. The obtained LiPSCl@LiOCl core@shell structure exhibits a synergistic effect. Consequently, compared with the bare LiPSCl, this composite electrolyte exhibits great performance improvements: 1) In Li|electrolyte|Li symmetric cells, the critical current density at 30 °C gets increased from 0.6 mA cm to 1.6 mA cm, and the lifetime gets prolonged from 320 h to 1400 h at the cycling current of 0.2 mA cm or from 6 h to 900 h at the cycling current of 0.5 mA cm; 2) In Li|electrolyte|NCM721 full cells running at 30 °C, the cycling capacity at 0.2 C (or 0.5 C) gets enhanced by 20% (or from unfeasible to be feasible) for 100 cycles and the rate capability reaches up to 2 C from 0.2 C; and in full cells running at 60 °C, the cycling capacity is increased by 7% at 0.2 C and the rate capability is enhanced to 3.0 C from 0.5 C. The experimental studies and theoretical computations show that the performance enhancements are due to the confined electron penetration and suppressed lithium dendrites growth at the LiPSCl@LiOCl interface.
由于具有高离子导电性、良好的可加工性和丰富的组成元素，LiPSCl 是开发全固态锂电池的理想硫化物-固体电解质（SSE）。然而，由于 LiPSCl/Li 界面的有害副反应以及 LiPSCl 相内锂枝晶的生长，其循环性较差。在此，我们报告了一种简单的界面工程补救方法，即在 LiPSCl 表面涂覆具有低电子传导性的锂兼容电解质 LiOCl，以提高其电化学性能。所获得的 LiPSCl@LiOCl 核@壳结构具有协同效应。因此，与裸 LiPSCl 相比，这种复合电解质的性能有了很大提高：1) 在锂|电解质|锂对称电池中，30 °C 时的临界电流密度从 0.6 mA cm 提高到 1.6 mA cm，循环电流为 0.2 mA cm 时的寿命从 320 h 延长到 1400 h，循环电流为 0.5 mA cm 时的寿命从 6 h 延长到 900 h；2) 在 30 °C 下运行的锂|电解质|NCM721 全电池中，0.2 C（或 0.实验研究和理论计算表明，性能的提高是由于在 LiPSCl@LiOCl 界面限制了电子的穿透并抑制了锂枝晶的生长。
{"title":"Synergistic Li6PS5Cl@Li3OCl composite electrolyte for high-performance all-solid-state lithium batteries","authors":"Yuzhe Zhang, Haolong Chang, Aiguo Han, Shijie Xu, Xinyu Wang, Shunjin Yang, Xiaohu Hu, Yujiang Sun, Xiao Sun, Xing Chen, Yongan Yang","doi":"10.1016/j.gee.2024.07.001","DOIUrl":"https://doi.org/10.1016/j.gee.2024.07.001","url":null,"abstract":"LiPSCl is a highly wanted sulfide-solid-electrolyte (SSE) for developing all-solid-state lithium batteries, due to its high ionic conductivity, good processability and abundant compositional elements. However, its cyclability is poor because of harmful side reactions at the LiPSCl/Li interface and growth of lithium dendrites inside LiPSCl phase. Herein, we report a simple interface-engineering remedy to boost the electrochemical performance of LiPSCl, by coating its surface with a Li-compatible electrolyte LiOCl having low electronic conductivity. The obtained LiPSCl@LiOCl core@shell structure exhibits a synergistic effect. Consequently, compared with the bare LiPSCl, this composite electrolyte exhibits great performance improvements: 1) In Li|electrolyte|Li symmetric cells, the critical current density at 30 °C gets increased from 0.6 mA cm to 1.6 mA cm, and the lifetime gets prolonged from 320 h to 1400 h at the cycling current of 0.2 mA cm or from 6 h to 900 h at the cycling current of 0.5 mA cm; 2) In Li|electrolyte|NCM721 full cells running at 30 °C, the cycling capacity at 0.2 C (or 0.5 C) gets enhanced by 20% (or from unfeasible to be feasible) for 100 cycles and the rate capability reaches up to 2 C from 0.2 C; and in full cells running at 60 °C, the cycling capacity is increased by 7% at 0.2 C and the rate capability is enhanced to 3.0 C from 0.5 C. The experimental studies and theoretical computations show that the performance enhancements are due to the confined electron penetration and suppressed lithium dendrites growth at the LiPSCl@LiOCl interface.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"24 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141586146","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}
Pub Date : 2024-06-29DOI: 10.1016/j.gee.2024.06.009
Yi Fang, Rui Ha, Jun Sun, Xue Liu, XiangDong Ding, WeiQun Shi
The separation of lithium isotopes (Li and Li) is of great importance for the nuclear industry. The lithium amalgam method is the only lithium isotopes separation process in industry, and the extensive use of mercury has raised concerns about its potential environmental hazards, which have prompted the search for more efficient and environmentally friendly alternatives. Crown ethers can bind lithium ions highly selectively and separate lithium isotopes effectively. A chemical exchange-based lithium isotopes separation method using crown ether decorated materials could be a viable and cost-effective alternative to the lithium amalgam method. In this review, we provide a systematic summary of the recent advances in lithium isotopes separation using crown ether decorated materials.
{"title":"Research progress on lithium isotopes separation by chemical exchange with crown ethers decorated materials","authors":"Yi Fang, Rui Ha, Jun Sun, Xue Liu, XiangDong Ding, WeiQun Shi","doi":"10.1016/j.gee.2024.06.009","DOIUrl":"https://doi.org/10.1016/j.gee.2024.06.009","url":null,"abstract":"The separation of lithium isotopes (Li and Li) is of great importance for the nuclear industry. The lithium amalgam method is the only lithium isotopes separation process in industry, and the extensive use of mercury has raised concerns about its potential environmental hazards, which have prompted the search for more efficient and environmentally friendly alternatives. Crown ethers can bind lithium ions highly selectively and separate lithium isotopes effectively. A chemical exchange-based lithium isotopes separation method using crown ether decorated materials could be a viable and cost-effective alternative to the lithium amalgam method. In this review, we provide a systematic summary of the recent advances in lithium isotopes separation using crown ether decorated materials.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"23 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141586147","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}
Pub Date : 2024-06-28DOI: 10.1016/j.gee.2024.06.007
Wenhao Jing, Zihao Jiao, Mengmeng Song, Ya Liu, Liejin Guo
Machine learning combined with density functional theory (DFT) enables rapid exploration of catalyst descriptors space such as adsorption energy, facilitating rapid and effective catalyst screening. However, there is still a lack of models for predicting adsorption energies on oxides, due to the complexity of elemental species and the ambiguous coordination environment. This work proposes an active learning workflow (LeNN) founded on local electronic transfer features () and the principle of coordinate rotation invariance. By accurately characterizing the electron transfer to adsorption site atoms and their surrounding geometric structures, LeNN mitigates abrupt feature changes due to different element types and clarifies coordination environments. As a result, it enables the prediction of ∗H adsorption energy on binary oxide surfaces with a mean absolute error (MAE) below 0.18 eV. Moreover, we incorporate local coverage () and leverage neutral network ensemble to establish an active learning workflow, attaining a prediction MAE below 0.2 eV for 5419 multi-∗H adsorption structures. These findings validate the universality and capability of the proposed features in predicting ∗H adsorption energy on binary oxide surfaces.
{"title":"An active learning workflow for predicting hydrogen atom adsorption energies on binary oxides based on local electronic transfer features","authors":"Wenhao Jing, Zihao Jiao, Mengmeng Song, Ya Liu, Liejin Guo","doi":"10.1016/j.gee.2024.06.007","DOIUrl":"https://doi.org/10.1016/j.gee.2024.06.007","url":null,"abstract":"Machine learning combined with density functional theory (DFT) enables rapid exploration of catalyst descriptors space such as adsorption energy, facilitating rapid and effective catalyst screening. However, there is still a lack of models for predicting adsorption energies on oxides, due to the complexity of elemental species and the ambiguous coordination environment. This work proposes an active learning workflow (LeNN) founded on local electronic transfer features () and the principle of coordinate rotation invariance. By accurately characterizing the electron transfer to adsorption site atoms and their surrounding geometric structures, LeNN mitigates abrupt feature changes due to different element types and clarifies coordination environments. As a result, it enables the prediction of ∗H adsorption energy on binary oxide surfaces with a mean absolute error (MAE) below 0.18 eV. Moreover, we incorporate local coverage () and leverage neutral network ensemble to establish an active learning workflow, attaining a prediction MAE below 0.2 eV for 5419 multi-∗H adsorption structures. These findings validate the universality and capability of the proposed features in predicting ∗H adsorption energy on binary oxide surfaces.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"40 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141549527","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}
Pub Date : 2024-06-27DOI: 10.1016/j.gee.2024.06.008
Sue-Faye Ng, Joel Jie Foo, Peipei Zhang, Steven Hao Wan Kok, Lling-Lling Tan, Binghui Chen, Wee-Jun Ong
Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides. Leveraging intrinsic heptazine/triazine phase and face-to-face contact, crystalline CN (CC3N5) was combined with protonated g-CN (pgCN) through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces. The highest photocatalytic performance was obtained through crystallinity and homojunction engineering, by controlling the pgCN:CC3N5 ratio. The 25:100 pgCN:CC3N5 homojunction (25CgCN) had the highest hydrogen production (1409.51 μmol h) and apparent quantum efficiency (25.04%, 420 nm), 8-fold and 180-fold higher than CC3N5 and pgCN, respectively. This photocatalytic homojunction improves benzaldehyde and hydrogen production activity, retaining 89% performance after 3 cycles (12 h) on a 3D-printed substrate. Electron paramagnetic resonance demonstrated higher ·OH, ·O and hole production of irradiated 25CgCN, attributed to crystallinity and homojunction interaction. Thus, electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.
{"title":"2D/2D homojunction-mediated charge separation: Synergistic effect of crystalline C3N5 and g-C3N4 via electrostatic self-assembly for photocatalytic hydrogen and benzaldehyde production","authors":"Sue-Faye Ng, Joel Jie Foo, Peipei Zhang, Steven Hao Wan Kok, Lling-Lling Tan, Binghui Chen, Wee-Jun Ong","doi":"10.1016/j.gee.2024.06.008","DOIUrl":"https://doi.org/10.1016/j.gee.2024.06.008","url":null,"abstract":"Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides. Leveraging intrinsic heptazine/triazine phase and face-to-face contact, crystalline CN (CC3N5) was combined with protonated g-CN (pgCN) through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces. The highest photocatalytic performance was obtained through crystallinity and homojunction engineering, by controlling the pgCN:CC3N5 ratio. The 25:100 pgCN:CC3N5 homojunction (25CgCN) had the highest hydrogen production (1409.51 μmol h) and apparent quantum efficiency (25.04%, 420 nm), 8-fold and 180-fold higher than CC3N5 and pgCN, respectively. This photocatalytic homojunction improves benzaldehyde and hydrogen production activity, retaining 89% performance after 3 cycles (12 h) on a 3D-printed substrate. Electron paramagnetic resonance demonstrated higher ·OH, ·O and hole production of irradiated 25CgCN, attributed to crystallinity and homojunction interaction. Thus, electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"10 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141549526","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}
With the increase of energy consumption, the shortage of fossil resource, and the aggravation of environmental pollution, the development of cost-effective and environmental friendly bio-based energy storage devices has become an urgent need. As the second most abundant natural polymer found in nature, lignin is mainly produced as the by-product of paper pulping and bio-refining industries. It possesses several inherent advantages, such as low-cost, high carbon content, abundant functional groups, and bio-renewable, making it an attractive candidate for the rechargeable battery material. Consequently, there has been a surge of research interest in utilizing lignin or lignin-based carbon materials as the components of lithium-ion (LIBs) or sodium-ion batteries (SIBs), including the electrode, binder, separator, and electrolyte. This review provides a comprehensive overview on the research progress of lignin-derived materials used in LIBs/SIBs, especially the application of lignin-based carbons as the anodes of LIBs/SIBs. The preparation methods and properties of lignin-derived materials with different dimensions are systemically discussed, which emphasizes on the relationship between the chemical/physical structures of lignin-derived materials and the performances of LIBs/SIBs. The current challenges and future prospects of lignin-derived materials in energy storage devices are also proposed.
{"title":"Research progress of lignin-derived materials in lithium/sodium ion batteries","authors":"Jingke Zhang, Hengxue Xiang, Zhiwei Cao, Shichao Wang, Meifang Zhu","doi":"10.1016/j.gee.2024.05.001","DOIUrl":"https://doi.org/10.1016/j.gee.2024.05.001","url":null,"abstract":"With the increase of energy consumption, the shortage of fossil resource, and the aggravation of environmental pollution, the development of cost-effective and environmental friendly bio-based energy storage devices has become an urgent need. As the second most abundant natural polymer found in nature, lignin is mainly produced as the by-product of paper pulping and bio-refining industries. It possesses several inherent advantages, such as low-cost, high carbon content, abundant functional groups, and bio-renewable, making it an attractive candidate for the rechargeable battery material. Consequently, there has been a surge of research interest in utilizing lignin or lignin-based carbon materials as the components of lithium-ion (LIBs) or sodium-ion batteries (SIBs), including the electrode, binder, separator, and electrolyte. This review provides a comprehensive overview on the research progress of lignin-derived materials used in LIBs/SIBs, especially the application of lignin-based carbons as the anodes of LIBs/SIBs. The preparation methods and properties of lignin-derived materials with different dimensions are systemically discussed, which emphasizes on the relationship between the chemical/physical structures of lignin-derived materials and the performances of LIBs/SIBs. The current challenges and future prospects of lignin-derived materials in energy storage devices are also proposed.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"4 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140932204","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}
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