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Efficient high-throughput screening for the preparation of propylene carbonate in a supercritical microchannel continuous flow system 在超临界微通道连续流系统中高效高通量筛选碳酸丙烯酯的制备方法
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102822
Yan Yang , Xiaotian Liu , Jingfu Jia , Haojia Chen , Xing Mao , Chao Xiong , Hongbing Ji

With the intensification of the global greenhouse effect, the utilization and fixation of CO2 has become one of the most important research fields in our world. However, there are still enormous challenges in achieving efficient fixation and conversion of carbon dioxide into high-value chemicals. Herein, the cycloaddition reaction strategy is adopted to achieve the fixation of supercritical carbon dioxide (SC-CO2) and the high-value conversion of carbon resources to propylene carbonate (PC) by using propylene oxide (PO) as the reaction precursor. Under tetrabutylammonium bromide (TBAB) as a catalyst and water (H2O) as a green solvent, the reaction factors, such as reaction temperature, reaction pressure, catalyst amount, water concentration and molar ratio of reactants, is conducted through the high-throughput screening technology to explore the catalytic performance in a self-designed microchannel reactor. The results indicate that the yield of PC can reach 91.82 % (along with a high selectivity of 99.12 %) at a reaction temperature of 160 ℃, reaction pressure of 8 MPa, catalyst amount of 0.72 mol %, reactants molar ratio of 8, and the residence time of 482 s. Besides, the thermodynamic and kinetic for carbonate synthesis are studied to fully understand the reaction process, and the activation energy of is explored. This work is more efficient than most similar reported works, which provide valuable insights into the practical application of CO2 in the supercritical state combined with microfluidics for synthesizing high-value monomers.

随着全球温室效应的加剧,二氧化碳的利用和固定已成为当今世界最重要的研究领域之一。然而,要实现二氧化碳的高效固定并转化为高价值的化学品仍面临巨大挑战。本文采用环化反应策略,以环氧丙烷(PO)为反应前驱体,实现超临界二氧化碳(SC-CO2)的固定和碳资源向碳酸丙烯酯(PC)的高值转化。在以四丁基溴化铵(TBAB)为催化剂、水(H2O)为绿色溶剂的条件下,通过高通量筛选技术,对反应温度、反应压力、催化剂用量、水浓度和反应物摩尔比等反应因素进行了研究,探讨了在自行设计的微通道反应器中的催化性能。结果表明,在反应温度为 160 ℃、反应压力为 8 MPa、催化剂用量为 0.72 mol %、反应物摩尔比为 8、停留时间为 482 s 的条件下,PC 的产率可达 91.82 %(选择性高达 99.12 %)。此外,还对碳酸盐合成的热力学和动力学进行了研究,以充分了解反应过程,并对活化能进行了探讨。这项工作比大多数类似报告的工作更有效率,为超临界状态下的二氧化碳与微流控技术相结合合成高价值单体的实际应用提供了宝贵的见解。
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引用次数: 0
Cycloaddition of limonene epoxide and CO2 over Zn/SBA-15 catalysts for limonene carbonate synthesis 在 Zn/SBA-15 催化剂上进行环氧化柠檬烯和 CO2 的环加成反应以合成碳酸柠檬烯酯
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102817
Carina Mosquera, Aída Luz Villa

The cycloaddition reaction of CO2 with epoxides such as limonene epoxide (LE) to form cyclic carbonates is considered a promising alternative for reducing CO2 emissions. In this work, CO2 fixation on LE to produce cyclic carbonates was carried out over Zn/SBA-15 with tetrabutylammonium bromide (TBAB) as co-catalyst and over NH3X-Zn/SBA-15 (X= Cl, Br, or I) catalysts. The catalysts were characterized by FT-IR, XRD, N2 adsorption–desorption isotherms, TEM, NH3-TPD, XPS, TGA and Py-FTIR. The Zn/SBA-15 support mainly presents Lewis’s acid sites of medium acidity; the surface area was 512 m2/g and 378 m2/g and the pore size were 9 nm and 7.2 nm, for Zn/SBA-15 and NH3Cl-Zn/SBA-15, respectively. The functionalization of Zn/SBA-15 was verified by FTIR, UV-vis, and XPS analysis. It was found that when Zn/SBA-15 was used as catalyst that reaction time had a significative effect on LE conversion and in the case of limonene carbonate selectivity, co-catalyst concentration variation had the main effect. Zn/SBA-15 catalyst can be reused up to 5 times without significant changes neither in conversion nor in limonene carbonate selectivity. The best LE conversion and limonene carbonate selectivity was 33% and 93%, respectively (1 M LE, 200 mg Zn/SBA-15, 7% TBAB; 30 bar, 18 h, 700 rpm and 20 mL diethyl carbonate). The reported catalytic system is a promising system for obtaining limonene carbonate using a heterogeneous catalyst.

二氧化碳与环氧化物(如环氧化柠檬烯(LE))发生环加成反应生成环状碳酸盐被认为是减少二氧化碳排放的一种有前途的替代方法。在这项工作中,以四丁基溴化铵(TBAB)为助催化剂的 Zn/SBA-15 和 NH3X-Zn/SBA-15(X= Cl、Br 或 I)催化剂上进行了二氧化碳固定在 LE 上生成环状碳酸盐的反应。催化剂的表征方法包括傅立叶变换红外光谱、X 射线衍射、N2 吸附-脱附等温线、TEM、NH3-TPD、XPS、TGA 和 Py-傅立叶变换红外光谱。Zn/SBA-15 和 NH3Cl-Zn/SBA-15 的比表面积分别为 512 m2/g 和 378 m2/g,孔径分别为 9 nm 和 7.2 nm。傅立叶变换红外光谱、紫外可见光和 XPS 分析验证了 Zn/SBA-15 的功能化。研究发现,使用 Zn/SBA-15 作为催化剂时,反应时间对 LE 转化率有显著影响,而在柠檬烯碳酸酯选择性方面,助催化剂浓度的变化具有主要影响。Zn/SBA-15 催化剂最多可重复使用 5 次,其转化率和碳酸柠檬烯选择性均无明显变化。最佳的 LE 转化率和柠檬烯碳酸酯选择性分别为 33% 和 93%(1 M LE、200 mg Zn/SBA-15、7% TBAB;30 bar、18 h、700 rpm 和 20 mL 碳酸二乙酯)。所报告的催化系统是一种利用异相催化剂获得碳酸柠檬烯的有前途的系统。
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引用次数: 0
A review of the application of wide-bandgap semiconductor photocatalysts for CO2 reduction 宽带隙半导体光催化剂在二氧化碳还原中的应用综述
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102808
Malathi Arumugam, Hsi-Hsien Yang

Artificial photosynthesis is a viable technique for mitigating the ever-increasing energy demands by converting carbon dioxide (CO2) into energy-rich C1 and C2+ products. A massive contribution to climate change and global warming is the widespread use of fossil fuels, responsible for more than 90% of total CO2 emissions and more than 75% of global greenhouse gas emissions. The most efficient method to convert CO2 into renewable and clean energy is utilizing plentiful sun energy to accelerate photo-induced chemical reactions. Practical CO2 reduction (CO2R), including choosing promising wide-bandgap (WBG) semiconductor photocatalysts with more negative conduction band potential, would be a holy grail for selective fuels and chemicals production. This review article deliberates on the importance of WBG semiconductor photocatalysts and a specific energy level in the conduction band for selective photocatalytic CO2R, which may assist in guiding future photocatalyst design for CO2R. In addition, the summary and prospects of WBG semiconductor photocatalysts and techniques for improving CO2 conversion efficiency and selectivity are discussed.

通过将二氧化碳(CO2)转化为富含能量的 C1 和 C2+ 产物,人工光合作用是缓解日益增长的能源需求的可行技术。化石燃料的广泛使用是造成气候变化和全球变暖的主要原因,其排放量占二氧化碳总排放量的 90% 以上,占全球温室气体排放量的 75% 以上。将二氧化碳转化为可再生清洁能源的最有效方法是利用充足的太阳能来加速光诱导化学反应。切实可行的二氧化碳还原(CO2R),包括选择具有更大负导带电位、前景广阔的宽带隙(WBG)半导体光催化剂,将是选择性燃料和化学品生产的圣杯。这篇综述文章探讨了 WBG 半导体光催化剂的重要性,以及选择性光催化 CO2R 在导带中的特定能级,这可能有助于指导未来 CO2R 光催化剂的设计。此外,文章还讨论了 WBG 半导体光催化剂的总结和前景,以及提高二氧化碳转化效率和选择性的技术。
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引用次数: 0
A bibliometric review on research progress, interest evolution and future trend in the field of recycled concrete by using CiteSpace (2004–2023) 利用 CiteSpace 对再生混凝土领域的研究进展、兴趣演变和未来趋势进行文献计量学审查(2004-2023 年)
IF 7.7 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102826
Li Lin-Bin , Yin Guang-Ji , Wen Xiao-Dong , Miao Ling , Zuo Xiao-Bao , Gao Xiao-Jian

The popularization of recycled concrete (RC) is an important way to achieve efficient resource utilization of construction solid waste (CSW), which can coordinate the sustainable economic development with environmental protection. In this paper, CiteSpace software is used to quantitatively analyze the literatures on RC field, identifying its research hotspots and recent developments. Based on the Web of Science database, we screened published literatures in the field of RC from 2004 to 2023, and obtained 2011 articles. CiteSpace software and knowledge graph technology are adopted to visually analyze the literature information, including the collaborators, keywords and citation status. The results show that, Xiao JZ from Tongji University, Poon CS from Hong Kong Polytechnic University and Tam VWY from University of Western Sydney publish a large number of articles and are frequently cited. It indicates that their researches are widely recognized in academic circles. There is a research team with a large size formed in the Chinese mainland, and the core members include Xiao JZ, Li WG, Chen ZP. At present, the research interest gradually shifts from recycled coarse aggregate to recycled fine aggregate, mainly focusing on microscale research of pore structure and interfacial transition zone. In addition, 8 co-citation clusters of selected references and the potential development trends are detailly analyzed. This study is helpful for researchers to fully understand the current hotspots and future research trends in the field of RC.

推广再生混凝土(RC)是实现建筑固体废弃物(CSW)高效资源化利用的重要途径,可协调经济可持续发展与环境保护的关系。本文利用 CiteSpace 软件对再生混凝土领域的文献进行定量分析,找出其研究热点和最新进展。基于 Web of Science 数据库,我们筛选了 2004 年至 2023 年 RC 领域发表的文献,共获得 2011 篇文章。采用CiteSpace软件和知识图谱技术对文献信息进行可视化分析,包括合作者、关键词和引用情况等。结果表明,同济大学的 Xiao JZ、香港理工大学的 Poon CS 和西悉尼大学的 Tam VWY 发表了大量文章,且被频繁引用。这表明他们的研究得到了学术界的广泛认可。中国大陆也形成了一支规模较大的研究团队,核心成员包括肖 JZ、李 WG、陈 ZP 等。目前,研究兴趣逐渐从再生粗骨料转向再生细骨料,主要集中在孔隙结构和界面过渡带的微观研究。此外,还详细分析了所选参考文献的 8 个共引集群及潜在发展趋势。本研究有助于研究人员全面了解再生骨料领域当前的研究热点和未来的研究趋势。
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引用次数: 0
Improving the performance of gliding arc plasma-catalytic dry reforming via a new post-plasma tubular catalyst bed 通过新型等离子后管式催化剂床提高滑弧等离子催化干重整的性能
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102820
Wencong Xu , Lukas C. Buelens , Vladimir V. Galvita , Annemie Bogaerts , Vera Meynen

A combination of a gliding arc plasmatron (GAP) reactor and a newly designed tubular catalyst bed (N-bed) was applied to investigate the post-plasma catalytic (PPC) effect for dry reforming of methane (DRM). As comparison, a traditional plasma catalyst bed (T-bed) was also utilized. The post-plasma catalytic effect of a Ni-based mixed oxide (Ni/MO) catalyst with a thermal catalytic performance of 77% CO2 and 86% CH4 conversion at 700 ℃ was studied. Although applying the T-bed had little effect on plasma based CO2 and CH4 conversion, an increase in selectivity to H2 was obtained with a maximum value of 89% at a distance of 2 cm. However, even when only α-Al2O3 packing material was used in the N-bed configuration, compared to the plasma alone and the T-bed, an increase of the CO2 and CH4 conversion from 53% and 53% to 69% and 69% to 83% was achieved. Addition of the Ni/MO catalyst further enhanced the DRM reaction, resulting in conversions of 79% for CO2 and 91% for CH4. Hence, although no insulation nor external heating was applied to the N-bed post plasma, it provides a slightly better conversion than the thermal catalytic performance with the same catalyst, while being fully electrically driven. In addition, an enhanced CO selectivity to 96% was obtained and the energy cost was reduced from ∼ 6 kJ/L (plasma alone) to 4.3 kJ/L. To our knowledge, it is the first time that a post-plasma catalytic system achieves this excellent catalytic performance for DRM without extra external heating or insulation.

研究人员将滑弧等离子体加速器(GAP)反应器和新设计的管式催化剂床(N-bed)相结合,研究了甲烷干转化(DRM)的后等离子体催化(PPC)效应。作为对比,还使用了传统的等离子催化剂床(T-bed)。研究了一种镍基混合氧化物(Ni/MO)催化剂的等离子体后催化效果,该催化剂在 700 ℃ 下的热催化性能为 77% 的 CO2 和 86% 的 CH4 转化率。虽然使用 T 型床对等离子体二氧化碳和甲烷的转化率影响不大,但在距离 2 厘米处,对 H2 的选择性增加,最大值为 89%。不过,即使在 N 型床配置中仅使用 α-Al2O3 填料,与单独使用等离子体和 T 型床相比,CO2 和 CH4 转化率也分别从 53% 和 53% 提高到 69% 和 69% 至 83%。添加 Ni/MO 催化剂进一步增强了 DRM 反应,使 CO2 和 CH4 的转化率分别达到 79% 和 91%。因此,虽然没有对 N-bed 后等离子体进行隔热或外部加热,但在完全电力驱动的情况下,其转化率略高于使用相同催化剂的热催化性能。此外,一氧化碳选择性提高到 96%,能源成本从 6 kJ/L(仅等离子体)降至 4.3 kJ/L。据我们所知,这是首次有一种后等离子体催化系统在没有额外外部加热或隔热的情况下为 DRM 实现如此优异的催化性能。
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引用次数: 0
Influence of morphology and composition of spherical layered double hydroxide particles and derived mixed oxides on photocatalytic CO2 reduction 球形层状双氢氧化物颗粒及其衍生混合氧化物的形态和组成对光催化还原二氧化碳的影响
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102810
Manuel Molina-Muriel , Mahesh Eledath-Changarath , Archit Dhingra , Josep Albero , Juan Francisco Sánchez-Royo , Antonio Ribera , Hermenegildo García

Considering the flexibility in the synthesis that allows the formation of materials with more than two metals, the present study reports the preparation of trimetallic layered double hydroxides (LDHs) having Al as structural tri-positive cation, Ti as photocatalytically active d0 transition metal and either Ni or Co as dipositive cation. In addition, these LDHs were used as precursors of the corresponding trimetallic mixed oxides (MO). LDH and MO materials in combination with Ru(bpy)3Cl2 as photosensitizer and triethanolamine as sacrificial electron donor were used as catalysts for CO2 reduction under solar light irradiation. A different product selectivity, either CH4 for Ni-LDH or CO and H2 for Co-MO, was observed with production rates for CH4 or CO that are among the highest reported for these systems. The role of the inorganic materials in the photocatalytic process was supported by transient absorption spectroscopy that revealed the quenching of the Ru(bpy)3Cl2 triplet excited state by Ni-LDH or Co-MO. An important finding was that the trimetallic Co-Ti-Al oxide with cobaltite structure is able to perform CO2 reduction in spite that the reduction potential of its conduction band is not sufficient to perform the process, evidence by photoluminescence revealing the existence of an upper electronic state responsible for the reduction. These results show the interest in screening multimetallic materials in photocatalysis due to their improved performance and diverse properties.

考虑到合成的灵活性,可以形成含有两种以上金属的材料,本研究报告了三金属层状双氢氧化物(LDHs)的制备方法,其中 Al 为结构性三阳离子,Ti 为光催化活性 d0 过渡金属,Ni 或 Co 为二阳离子。此外,这些 LDHs 还被用作相应的三金属混合氧化物(MO)的前驱体。LDH 和 MO 材料与作为光敏剂的 Ru(bpy)3Cl2 和作为牺牲电子供体的三乙醇胺相结合,被用作催化剂在太阳光照射下还原 CO2。观察到了不同的产物选择性,Ni-LDH 为 CH4,Co-MO 为 CO 和 H2。无机材料在光催化过程中的作用得到了瞬态吸收光谱的支持,该光谱显示了 Ni-LDH 或 Co-MO 对 Ru(bpy)3Cl2 三重激发态的淬灭。一个重要的发现是,具有钴酸盐结构的三金属 Co-Ti-Al 氧化物能够进行二氧化碳还原,尽管其导带的还原电位不足以完成这一过程,光致发光证明存在一个负责还原的上层电子态。这些结果表明,在光催化过程中筛选多金属材料很有意义,因为它们具有更好的性能和多样化的特性。
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引用次数: 0
Novel wastewater recovery process for sustainable sodium carbonate production with CO2 and SOx utilization 利用二氧化碳和硫氧化物可持续生产碳酸钠的新型废水回收工艺
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102824
Jongdu Choi , Jonghun Lim , Yurim Kim , Seongbin Ga , Junghwan Kim

Ammonia-soda process, which produce soda ash, emits flue gas containing a large amount of CO2 and SOx. The wastewater discharged from the ammonia-soda process contains cations, such as Na+ and Ca2+, which can be recovered and reacted with a CO2 and SOx. In this study, we designed a CO2 and SOx utilization process for the sustainable production of sodium carbonate using wastewater recovery system, extracting Na+ and Ca2+. The proposed process involved the following steps: (1) metal-ion separation, which produces NaOH and Ca(OH)2; (2) capture and utilization of SOx using Ca(OH)2; and (3) capture and utilization of CO2 using NaOH and Ca(OH)2, respectively. The economic feasibility of the proposed process was verified by comparing its total annualized cost (TAC) with those of conventional processes. Approximately 99% of SOx was captured to produce high-purity desulfurized gypsum, and 99% of CO2 was captured to be transformed into CaCO3. To confirm the CO2 reduction of the process, the carbon dioxide equivalent (CO2e) was calculated by evaluating the amount of greenhouse gases. The CO2e decreased to 71.4% compared with that of the conventional process. The TAC of the proposed process decreased by 10.67% and 19.63% compared with that of the ammonia-soda and Hou processes, respectively. Thus, this study proposes an industrially potential process design for sustainable sodium carbonate production by utilizing CO2 and SOx with wastewater recycling, without additional reactants, making it more economically viable.

氨碱法生产纯碱,排放的烟气中含有大量二氧化碳和硫氧化物。氨碱法排放的废水中含有 Na+ 和 Ca2+ 等阳离子,这些阳离子可以回收并与 CO2 和 SOx 反应。在这项研究中,我们设计了一种二氧化碳和硫氧化物利用工艺,利用废水回收系统提取 Na+ 和 Ca2+,实现碳酸钠的可持续生产。拟议工艺包括以下步骤:(1) 金属离子分离,产生 NaOH 和 Ca(OH)2;(2) 利用 Ca(OH)2 捕获和利用 SOx;(3) 利用 NaOH 和 Ca(OH)2 分别捕获和利用 CO2。通过比较拟议工艺与传统工艺的总年化成本(TAC),验证了拟议工艺的经济可行性。约 99% 的硫氧化物被捕获,用于生产高纯度脱硫石膏,99% 的 CO2 被捕获,转化为 CaCO3。为了证实该工艺的二氧化碳减排效果,通过评估温室气体的数量计算出了二氧化碳当量(CO2e)。与传统工艺相比,二氧化碳当量减少了 71.4%。与氨-碱工艺和侯工艺相比,拟议工艺的 TAC 分别减少了 10.67% 和 19.63%。因此,本研究提出了一种具有工业潜力的可持续碳酸钠生产工艺设计,通过废水回收利用 CO2 和 SOx,无需额外的反应物,使其更具经济可行性。
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引用次数: 0
Fresh, hardened, durability and microstructure properties of seawater concrete: A systematic review 海水混凝土的新鲜、硬化、耐久性和微观结构特性:系统综述
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102815
Abdeliazim Mustafa Mohamed , Bassam A. Tayeh , Samadar S. Majeed , Yazan Issa Abu Aisheh , Musab Nimir Ali Salih

Seawater concrete (SWC) is an environmentally friendly construction material that addresses freshwater scarcity concerns by utilising seawater as a mixing water source. This review study comprehensively examines SWC by focusing on its fresh properties, hardened properties, seawater composition, microstructure and porosity, hydration process, durability, test methods and electrical resistivity. The study analyses the influence of additives and admixtures on SWC’s performance by considering constituents such as cement, aggregates and seawater. It also explores the impact of manufacturing techniques, including mix design. The potential of SWC is revealed and compared with that of conventional concrete by evaluating and comparing their mechanical properties, such as compressive strength, modulus of elasticity, stress-strain behaviours, tensile strength and flexural strength. This study primarily aims to thoroughly examine the characteristics of SWC in its fresh and hardened states. It also assesses the advantages and drawbacks of seawater as a mixing water source. Moreover, this study delves into the impact of seawater composition on crucial aspects, such as the hydration process, microstructure and porosity of concrete. It also used various test methods to explore SWC durability, including resistance to chloride ingress, sulphate attack and carbonation. Furthermore, the importance of electrical resistivity for corrosion prevention is discussed in this study. The carbon-negative cement production and carbonation curing of seawater concrete underscore groundbreaking advancements, emphasizing sustainability and climate mitigation in the construction industry. Overall, this study aims to enhance the comprehension of SWC and provide valuable insights for engineers, researchers and policymakers in concrete technology.

海水混凝土(SWC)是一种环保型建筑材料,它利用海水作为混合水源,解决了淡水稀缺的问题。本综述研究全面考察了海水混凝土的新拌性能、硬化性能、海水成分、微观结构和孔隙率、水化过程、耐久性、测试方法和电阻率。研究通过考虑水泥、集料和海水等成分,分析了添加剂和掺合料对深水泥浆性能的影响。研究还探讨了制造技术(包括混合设计)的影响。通过评估和比较抗压强度、弹性模量、应力-应变行为、抗拉强度和抗折强度等力学性能,揭示了深层螺旋岩混凝土的潜力,并将其与传统混凝土进行比较。本研究的主要目的是深入研究新拌混凝土和硬化混凝土的特性。它还评估了海水作为混合水源的优点和缺点。此外,本研究还深入探讨了海水成分对混凝土水化过程、微观结构和孔隙率等关键方面的影响。研究还采用各种测试方法来探讨海水混凝土的耐久性,包括抗氯化物侵入、硫酸盐侵蚀和碳化的能力。此外,本研究还讨论了电阻率对防腐蚀的重要性。负碳水泥的生产和海水混凝土的碳化养护凸显了突破性进展,强调了建筑行业的可持续性和气候减缓。总之,本研究旨在加深对海水混凝土的理解,并为混凝土技术领域的工程师、研究人员和决策者提供有价值的见解。
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引用次数: 0
Production of polyhydroxybutyrate from industrial flue gas by microbial electrosynthesis 利用微生物电合成法从工业烟气中生产聚羟基丁酸盐
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102800
Alexander Langsdorf , Julian Philipp Schütz , Roland Ulber , Markus Stöckl , Dirk Holtmann

The aim of this work was to produce the biopolymer polyhydroxybutyrate (PHB) from industrial flue gas as CO2 source and electrolysis originating hydrogen via microbial electrosynthesis. Besides the laboratory experiments, the experiments were carried out under industrial conditions directly on-site in a cogeneration plant. We were able to demonstrate that the use of flue gas as a CO2 source has no detectable negative effect on bacterial growth and PHB production in comparison to a pure gas mixture. In an electrochemical H-cell 333 ± 44 mg L−1 PHB were obtained, which corresponds to a PHB content of 43 ± 3 % of the cell dry weight. By using flue gas for the production of the biopolymer PHB, not only CO2 emissions are reduced, but also possible environmental pollution from non-biodegradable plastics. To the best of our knowledge, this is the first time that the production of PHB from flue gas has been demonstrated using Cupriavidus necator.

这项工作的目的是以工业烟气为二氧化碳源,通过微生物电合成法电解氢气,生产生物聚合物聚羟基丁酸(PHB)。除实验室实验外,我们还在热电联产厂现场直接进行了工业条件下的实验。我们能够证明,与纯混合气体相比,使用烟道气作为二氧化碳源对细菌的生长和 PHB 的生产没有任何负面影响。在电化学 H 细胞中获得了 333 ± 44 mg L-1 PHB,相当于细胞干重的 43 ± 3 %。通过使用烟道气生产生物聚合物 PHB,不仅减少了二氧化碳排放量,还减少了不可降解塑料可能造成的环境污染。据我们所知,这是首次证明利用烟道气生产 PHB 是可行的。
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引用次数: 0
Theoretical performance optimization of enzymatic electrochemical CO2 reduction to formate: Voltage, concentration, temperature, pressure, and flow rate 酶电化学二氧化碳还原甲酸盐的理论性能优化:电压、浓度、温度、压力和流速
IF 7.7 2区 工程技术 Q1 Chemical Engineering Pub Date : 2024-05-01 DOI: 10.1016/j.jcou.2024.102805
Daniel Moreno

Formic acid (FA) is a notable fuel product due to its atom economy, low activation energy, and applications in flow cells and hydrogen storage. While metal catalysts are typically used, selectivity remains a challenge. Here, an enzymatic catalyst is employed to selectively convert CO2 to FA as formate. This study documents the development of a computational model to examine the conversion of CO2 to formate under a wide range of conditions. The model examines the electrochemical reduction of a charge carrier, ethyl viologen (EV), and its subsequent use in an enzymatic catalyst to convert CO2 and protons in solution to formate. The model was first developed for a small-scale batch reactor, then later expanded to a dual-cell flow system, where the reduction of EV and production of formate are kept in separated cells, and flow rate is introduced as an additional variable parameter. While no studies have directly used all parameters addressed in the computations presented here, many of the conditions selected align with what has previously been used in experiments, and similar production rates and efficiencies are obtained. The most challenging parameters to study were charge carrier concentration and applied voltage, which showed optimal ranges in the cases studied for the batch and flow cell. While the study gives guidance toward which conditions would be favored experimentally to increase production rate and efficiency experimental studies should nonetheless be run at suggested optimal conditions to better adapt parameters made in both models.

甲酸(FA)因其原子经济性、低活化能以及在流动电池和储氢中的应用而成为一种著名的燃料产品。虽然通常使用金属催化剂,但选择性仍然是一个挑战。本研究采用酶催化剂将二氧化碳选择性地转化为甲酸甲酯。本研究记录了一个计算模型的开发过程,该模型用于研究在各种条件下将 CO2 转化为甲酸盐的过程。该模型研究了电荷载体乙基紫精(EV)的电化学还原过程,以及随后利用酶催化剂将溶液中的二氧化碳和质子转化为甲酸盐的过程。该模型最初是为一个小规模间歇式反应器开发的,后来扩展到一个双池流动系统,在该系统中,EV 的还原和甲酸盐的生成是在分离的池中进行的,并且引入了流速作为额外的可变参数。虽然没有任何研究直接使用了本文计算中涉及的所有参数,但所选的许多条件与之前实验中使用的条件一致,并获得了类似的生产率和效率。研究中最具挑战性的参数是电荷载流子浓度和外加电压,这两个参数在所研究的间歇式和流动池中均显示出最佳范围。虽然这项研究提供了实验条件方面的指导,以提高生产率和效率,但实验研究仍应在建议的最佳条件下进行,以便更好地调整两种模型中的参数。
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引用次数: 0
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Journal of CO2 Utilization
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