EES catalysis最新文献

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Rational element-doping of FeOOH-based electrocatalysts for efficient ammonia electrosynthesis† 合理元素掺杂feooh基电催化剂用于高效氨电合成
EES catalysis Pub Date : 2023-11-01 DOI: 10.1039/D3EY00208J
Haifan Wang, Menglei Yuan, Jingxian Zhang, Yiling Bai, Ke Zhang, Bin Li and Guangjin Zhang
{"title":"Rational element-doping of FeOOH-based electrocatalysts for efficient ammonia electrosynthesis†","authors":"Haifan Wang, Menglei Yuan, Jingxian Zhang, Yiling Bai, Ke Zhang, Bin Li and Guangjin Zhang","doi":"10.1039/D3EY00208J","DOIUrl":"10.1039/D3EY00208J","url":null,"abstract":"<p >Electrocatalysis has been intensively studied in nitrogen (N<small><sub>2</sub></small>) reduction for its sustainable power and stable catalytic performance, but it is still limited by weak activation of N<small><sub>2</sub></small> at the catalytic sites, and the competition from the hydrogen evolution reaction (HER). The special d-orbital electron arrangement of transition metals and the tuning of the microenvironment provide possible strategies to enhance the activation of N<small><sub>2</sub></small>, while improving the selectivity of the eNRR. Herein, FeO(OH, S) with high spin state and Mo–FeOOH with low spin state were designed around the FeOOH-based catalysts through elemental doping, which could achieve excellent ammonia yield performance of 80.1 ± 4.0 μg h<small><sup>−1</sup></small> mg<small><sub>cat</sub></small><small><sup>−1</sup></small> (FE 36.9 ± 0.5%) and 86.8 ± 4.1 μg h<small><sup>−1</sup></small> mg<small><sub>cat</sub></small><small><sup>−1</sup></small> (FE 29.1 ± 0.8%) in 0.1 M LiClO<small><sub>4</sub></small> at −0.6 V <em>vs.</em> RHE, respectively, coupled with polyethylene glycol (PEG) to inhibit the HER. Based on theoretical calculations to investigate the adsorption of N<small><sub>2</sub></small> on Fe sites, the FeO(OH, S) catalyst has stronger adsorption ability, which may originate from the high spin effect, which means that the more isolated and highly active e<small><sub>g</sub></small> orbital electrons are more beneficial to realize the electronic feedback mechanism, promoting the d–π* orbital interaction with N<small><sub>2</sub></small>.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 324-334"},"PeriodicalIF":0.0,"publicationDate":"2023-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00208j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138515493","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cobalt-free layered perovskites RBaCuFeO5+δ (R = 4f lanthanide) as electrocatalysts for the oxygen evolution reaction† 无钴层状钙钛矿RBaCuFeO5+δ (R = 4f镧系)作为析氧反应的电催化剂
EES catalysis Pub Date : 2023-10-31 DOI: 10.1039/D3EY00142C
Elena Marelli, Jike Lyu, Mickaël Morin, Maxime Leménager, Tian Shang, N. Sena Yüzbasi, Dino Aegerter, Jinzhen Huang, Niéli D. Daffé, Adam H. Clark, Denis Sheptyakov, Thomas Graule, Maarten Nachtegaal, Ekaterina Pomjakushina, Thomas J. Schmidt, Matthias Krack, Emiliana Fabbri and Marisa Medarde
{"title":"Cobalt-free layered perovskites RBaCuFeO5+δ (R = 4f lanthanide) as electrocatalysts for the oxygen evolution reaction†","authors":"Elena Marelli, Jike Lyu, Mickaël Morin, Maxime Leménager, Tian Shang, N. Sena Yüzbasi, Dino Aegerter, Jinzhen Huang, Niéli D. Daffé, Adam H. Clark, Denis Sheptyakov, Thomas Graule, Maarten Nachtegaal, Ekaterina Pomjakushina, Thomas J. Schmidt, Matthias Krack, Emiliana Fabbri and Marisa Medarde","doi":"10.1039/D3EY00142C","DOIUrl":"10.1039/D3EY00142C","url":null,"abstract":"<p >Co-based perovskite oxides are intensively studied as promising catalysts for electrochemical water splitting in an alkaline environment. However, the increasing Co demand by the battery industry is pushing the search for Co-free alternatives. Here we report a systematic study of the Co-free layered perovskite famil<em>y</em> RBaCuFeO<small><sub>5+<em>δ</em></sub></small> (R = 4f lanthanide), where we uncover the existence of clear correlations between electrochemical properties and several physicochemical descriptors. Using a combination of advanced neutron and X-ray synchrotron techniques with <em>ab initio</em> DFT calculations we demonstrate and rationalize the positive impact of a large R ionic radius in their oxygen evolution reaction (OER) activity. We also reveal that, in these materials, Fe<small><sup>3+</sup></small> is the transition metal cation the most prone to donate electrons. We also show that similar R<small><sup>3+</sup></small>/Ba<small><sup>2+</sup></small> ionic radii favor the incorporation and mobility of oxygen in the layered perovskite structure and increase the number of available O diffusion paths, which have an additional, positive impact on both, the electric conductivity and the OER process. An unexpected result is the observation of a clear surface reconstruction exclusively in oxygen-rich samples (<em>δ</em> &gt; 0), a fact that could be related to their superior OER activity. The encouraging intrinsic OER values obtained for the most active electrocatalyst (LaBaCuFeO<small><sub>5.49</sub></small>), together with the possibility of industrially producing this material in nanocrystalline form should inspire the design of other Co-free oxide catalysts with optimal properties for electrochemical water splitting.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 335-350"},"PeriodicalIF":0.0,"publicationDate":"2023-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00142c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138515489","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Multidisciplinary approaches for enzyme biocatalysis in pharmaceuticals: protein engineering, computational biology, and nanoarchitectonics 制药中的酶生物催化多学科方法:蛋白质工程学、计算生物学和纳米结构学
EES catalysis Pub Date : 2023-10-28 DOI: 10.1039/D3EY00239J
Suhyeon Kim, Seongmin Ga, Hayeon Bae, Ronald Sluyter, Konstantin Konstantinov, Lok Kumar Shrestha, Yong Ho Kim, Jung Ho Kim and Katsuhiko Ariga
{"title":"Multidisciplinary approaches for enzyme biocatalysis in pharmaceuticals: protein engineering, computational biology, and nanoarchitectonics","authors":"Suhyeon Kim, Seongmin Ga, Hayeon Bae, Ronald Sluyter, Konstantin Konstantinov, Lok Kumar Shrestha, Yong Ho Kim, Jung Ho Kim and Katsuhiko Ariga","doi":"10.1039/D3EY00239J","DOIUrl":"10.1039/D3EY00239J","url":null,"abstract":"<p >Enzyme biocatalysis is reshaping pharmaceutical synthesis, offering sustainable and efficient pathways for drug discovery and production. This paradigm shift towards eco-friendly methodologies addresses concerns inherent in traditional chemical synthesis. Enzymes, celebrated for their precision and adaptability to mild conditions, are poised as ideal candidates for pharmaceutical applications. Their versatility facilitates the synthesis of diverse pharmaceutical compounds, ensuring precise drug design and minimizing environmental impact. The integration of multidisciplinary approaches, including protein engineering, computational biology, and nanoarchitectonics, holds the potential to propel enzyme biocatalysis even further. Protein engineering utilizes directed evolution and rational design to customize enzymes, enhancing their stability and efficacy. Computational biology aids in deciphering enzymatic mechanisms, while nanoarchitectonics introduces innovative enzyme integration strategies into continuous flow systems. This comprehensive review explores how these multidisciplinary approaches can revolutionize pharmaceutical research and production. The synergy among these disciplines promises to expedite pharmaceutical processes, promote sustainability, optimize efficiency, and elevate precision—aligning perfectly with the evolving requirements of the pharmaceutical industry.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 14-48"},"PeriodicalIF":0.0,"publicationDate":"2023-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00239j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134883771","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Operando insights into correlating CO coverage and Cu–Au alloying with the selectivity of Au NP-decorated Cu2O nanocubes during the electrocatalytic CO2 reduction† 在电催化二氧化碳还原过程中将一氧化碳覆盖率和铜金合金化与金氮氧化物装饰的氧化铜纳米立方体的选择性联系起来的操作性见解†.
EES catalysis Pub Date : 2023-10-25 DOI: 10.1039/D3EY00162H
Clara Rettenmaier, Antonia Herzog, Daniele Casari, Martina Rüscher, Hyo Sang Jeon, David Kordus, Mauricio Lopez Luna, Stefanie Kühl, Uta Hejral, Earl M. Davis, See Wee Chee, Janis Timoshenko, Duncan T.L. Alexander, Arno Bergmann and Beatriz Roldan Cuenya
{"title":"Operando insights into correlating CO coverage and Cu–Au alloying with the selectivity of Au NP-decorated Cu2O nanocubes during the electrocatalytic CO2 reduction†","authors":"Clara Rettenmaier, Antonia Herzog, Daniele Casari, Martina Rüscher, Hyo Sang Jeon, David Kordus, Mauricio Lopez Luna, Stefanie Kühl, Uta Hejral, Earl M. Davis, See Wee Chee, Janis Timoshenko, Duncan T.L. Alexander, Arno Bergmann and Beatriz Roldan Cuenya","doi":"10.1039/D3EY00162H","DOIUrl":"10.1039/D3EY00162H","url":null,"abstract":"<p >Electrochemical reduction of CO<small><sub>2</sub></small> (CO<small><sub>2</sub></small>RR) is an attractive technology to reintegrate the anthropogenic CO<small><sub>2</sub></small> back into the carbon cycle driven by a suitable catalyst. This study employs highly efficient multi-carbon (C<small><sub>2+</sub></small>) producing Cu<small><sub>2</sub></small>O nanocubes (NCs) decorated with CO-selective Au nanoparticles (NPs) to investigate the correlation between a high CO surface concentration microenvironment and the catalytic performance. Structure, morphology and near-surface composition are studied <em>via operando</em> X-ray absorption spectroscopy and surface-enhanced Raman spectroscopy, <em>operando</em> high-energy X-ray diffraction as well as quasi <em>in situ</em> X-ray photoelectron spectroscopy. These <em>operando</em> studies show the continuous evolution of the local structure and chemical environment of our catalysts during reaction conditions. Along with its alloy formation, a CO-rich microenvironment as well as weakened average CO binding on the catalyst surface during CO<small><sub>2</sub></small>RR is detected. Linking these findings to the catalytic function, a complex compositional interplay between Au and Cu is revealed in which higher Au loadings primarily facilitate CO formation. Nonetheless, the strongest improvement in C<small><sub>2+</sub></small> formation appears for the lowest Au loadings, suggesting a beneficial role of the Au–Cu atomic interaction for the catalytic function in CO<small><sub>2</sub></small>RR. This study highlights the importance of site engineering and <em>operando</em> investigations to unveil the electrocatalyst's adaptations to the reaction conditions, which is a prerequisite to understand its catalytic behavior.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 311-323"},"PeriodicalIF":0.0,"publicationDate":"2023-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00162h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135212409","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Research progress and perspectives on photocatalysts based on the lead-free double halide perovskite 基于无铅双卤化物过氧化物的光催化剂的研究进展与展望
EES catalysis Pub Date : 2023-10-23 DOI: 10.1039/D3EY00229B
Do Yeon Heo, Mahider Asmare Tekalgne and Soo Young Kim
{"title":"Research progress and perspectives on photocatalysts based on the lead-free double halide perovskite","authors":"Do Yeon Heo, Mahider Asmare Tekalgne and Soo Young Kim","doi":"10.1039/D3EY00229B","DOIUrl":"10.1039/D3EY00229B","url":null,"abstract":"<p >Photocatalytic technology stands as a promising solution to address the current energy and environmental challenges. Halide perovskites, particularly lead-free double halide perovskites, have garnered recognition as next-generation photocatalysts due to their adjustable bandgap, low binding energy, broad visible light absorption range, and efficient charge carrier transfer. In this review, we explore the utilization of lead-free double halide perovskites characterized by their non-toxic attributes and diverse chemical compositions and properties as photocatalysts for both hydrogen production and carbon dioxide reduction. We commence by presenting an overview of lead-free double halide perovskites, followed by a comprehensive analysis of recent research outcomes pertaining to their application as photocatalysts for hydrogen production and carbon dioxide reduction. Lastly, we discuss the challenges and prospects associated with lead-free double halide perovskite photocatalysts. This review is anticipated to serve as a valuable reference for the development of lead-free double halide perovskite-based photocatalysts, addressing critical aspects in the pursuit of achieving high-efficiency hydrogen generation and carbon dioxide reduction, crucial for our future energy and environmental needs.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 94-108"},"PeriodicalIF":0.0,"publicationDate":"2023-10-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00229b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135152839","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Harnessing single-atom catalysts for CO2 electroreduction: a review of recent advances 利用单原子催化剂进行二氧化碳电还原:最新进展综述
EES catalysis Pub Date : 2023-10-13 DOI: 10.1039/D3EY00150D
Chang Chen, Jiazhan Li, Xin Tan, Yu Zhang, Yifan Li, Chang He, Zhiyuan Xu, Chao Zhang and Chen Chen
{"title":"Harnessing single-atom catalysts for CO2 electroreduction: a review of recent advances","authors":"Chang Chen, Jiazhan Li, Xin Tan, Yu Zhang, Yifan Li, Chang He, Zhiyuan Xu, Chao Zhang and Chen Chen","doi":"10.1039/D3EY00150D","DOIUrl":"10.1039/D3EY00150D","url":null,"abstract":"<p >Electrochemical CO<small><sub>2</sub></small> reduction is an effective pathway to convert CO<small><sub>2</sub></small> into valuable fuels and chemicals, which provides a potential alternative to fossil fuel resources and plays a notable role in mitigating environmental issues and energy crises. The feasibility of the CO<small><sub>2</sub></small> reduction reaction (CO<small><sub>2</sub></small>RR) hinges on the development of catalysts that feature high activity, selectivity, and stability. As a new research frontier, single-atom catalysts (SACs) have shown immense potential in the field of CO<small><sub>2</sub></small> reduction by virtue of their unique geometric/electronic structures, and have also provided new opportunities for atomic-level understanding of structure–function relationships. Therefore, this review aims to outline recent advances of SACs for CO<small><sub>2</sub></small>RR. We start by introducing the current research status and general synthesis strategies of SACs, and then shift our focus to analyzing the various regulation strategies and deciphering the structure–function relationships of SACs in the CO<small><sub>2</sub></small>RR. Finally, we propose future directions and opportunities for CO<small><sub>2</sub></small>RR-oriented SACs, while also highlighting potential challenges that may be encountered along the way.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 71-93"},"PeriodicalIF":0.0,"publicationDate":"2023-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00150d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136304871","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Boosting the catalytic performance of metal–zeolite catalysts in the hydrocracking of polyolefin wastes by optimizing the nanoscale proximity† 通过优化纳米级接近度† 提高金属沸石催化剂在聚烯烃废料加氢裂化中的催化性能
EES catalysis Pub Date : 2023-10-09 DOI: 10.1039/D3EY00180F
Xinlei Han, Xinru Zhou, Tuo Ji, Feng Zeng, Weiping Deng, Zhenchen Tang and Rizhi Chen
{"title":"Boosting the catalytic performance of metal–zeolite catalysts in the hydrocracking of polyolefin wastes by optimizing the nanoscale proximity†","authors":"Xinlei Han, Xinru Zhou, Tuo Ji, Feng Zeng, Weiping Deng, Zhenchen Tang and Rizhi Chen","doi":"10.1039/D3EY00180F","DOIUrl":"10.1039/D3EY00180F","url":null,"abstract":"<p >Hydrocracking polyolefins using bifunctional metal–zeolite catalysts is a pivotal strategy for the catalytic upcycling of plastic waste to produce value-added fuels. However, the macro-molecular size and stable C–C bond of polyolefins impose major challenges on catalyst design based on noble metal and microporous zeolites. The lack of investigation into the nanoscale proximity between Pt and USY has hindered the development of an evolving generation of catalysts. Herein, we report Pt/USY prepared by colloid-immobilization method with Pt nanoparticles exclusively located on the surface of USY is a superior catalyst (&gt;50% higher activity) compared to its analogues that have Pt inside or away from USY crystalline, reaching a selectivity to gasoline (C<small><sub>5–12</sub></small>) over 90%. The formation rate of liquid products reaches 6122 g<small><sub>liquid</sub></small> g<small><sub>Pt</sub></small><small><sup>−1</sup></small> h<small><sup>−1</sup></small> and 5048 g<small><sub>liquid</sub></small> g<small><sub>Pt</sub></small><small><sup>−1</sup></small> h<small><sup>−1</sup></small> in hydrocracking polyethylene (PE) and polypropylene (PP) at 280 °C, respectively. The hydrocracking of model alkanes with different molecular sizes demonstrates the nanoscale Pt-USY proximity as a key criterion in optimizing the accessibility and acidic environment of Pt, and the diffusion distance between metal and acid sites. These findings comprise a significant step forward toward rational catalyst design aiming at upcycling plastic waste for sustainable fuel production.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 300-310"},"PeriodicalIF":0.0,"publicationDate":"2023-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00180f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136202105","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Highly selective Ag foam gas diffusion electrodes for CO2 electroreduction by pulsed hydrogen bubble templation† 采用脉冲氢泡模板制备的高选择性银泡沫气体扩散电极用于CO2电还原
EES catalysis Pub Date : 2023-10-09 DOI: 10.1039/D3EY00220A
Hendrik Hoffmann, Maximilian Kutter, Jens Osiewacz, Melanie-Cornelia Paulisch-Rinke, Steffen Lechner, Barbara Ellendorff, Annika Hilgert, Ingo Manke, Thomas Turek and Christina Roth
{"title":"Highly selective Ag foam gas diffusion electrodes for CO2 electroreduction by pulsed hydrogen bubble templation†","authors":"Hendrik Hoffmann, Maximilian Kutter, Jens Osiewacz, Melanie-Cornelia Paulisch-Rinke, Steffen Lechner, Barbara Ellendorff, Annika Hilgert, Ingo Manke, Thomas Turek and Christina Roth","doi":"10.1039/D3EY00220A","DOIUrl":"10.1039/D3EY00220A","url":null,"abstract":"<p >The electrochemical reduction of carbon dioxide to valuable fossil-free products opens up a way to close the carbon cycle, if based solely on renewable energy sources. Making the process industrially viable, however, needs high CO<small><sub>2</sub></small> conversion rates, efficient electrodes, and high selectivity for desired products. To reach this goal, highly catalytically active porous electrodes with maximized surface areas are required. We combined pulsed electrochemical deposition of the Ag foam catalyst with ionomer infiltration of the electrode to produce Ag-based gas diffusion electrodes (GDEs) in a facile and fast production process. Using the dynamic hydrogen bubble templation method (DHBT), we utilized the parasitic hydrogen evolution reaction (HER) to aid the solvent free structuring of the 3D catalyst network and directly manufacture a GDE. Different deposition parameters and in particular pulse-to-pause ratios increased the amount of deposited catalyst and successfully reduced the overpotential during CO<small><sub>2</sub></small>RR operation. To inhibit electrode flooding and decrease CO<small><sub>2</sub></small> mass transport limitations during CO<small><sub>2</sub></small>RR, we further infiltrated the electrode with a suitable perfluorosulfonic acid ionomer. SEM and EDS analyses showed a homogeneous Ag/F distribution along the cross section of the electrodes. These electrodes catalyzed the conversion of CO<small><sub>2</sub></small> to CO at industrially viable current densities of 500 mA cm<small><sup>−2</sup></small> with an unprecedented faradaic efficiency up to 76% in 1 M KHCO<small><sub>3</sub></small>.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 286-299"},"PeriodicalIF":0.0,"publicationDate":"2023-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00220a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519295","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Single atom catalysts for water electrolysis: from catalyst-coated substrate to catalyst-coated membrane 水电解用单原子催化剂:从涂覆催化剂的底物到涂覆催化剂的膜
EES catalysis Pub Date : 2023-10-05 DOI: 10.1039/D3EY00165B
Sol A Lee, Sang Eon Jun, Sun Hwa Park, Ki Chang Kwon, Jong Hun Kang, Min Sang Kwon and Ho Won Jang
{"title":"Single atom catalysts for water electrolysis: from catalyst-coated substrate to catalyst-coated membrane","authors":"Sol A Lee, Sang Eon Jun, Sun Hwa Park, Ki Chang Kwon, Jong Hun Kang, Min Sang Kwon and Ho Won Jang","doi":"10.1039/D3EY00165B","DOIUrl":"10.1039/D3EY00165B","url":null,"abstract":"<p >Green hydrogen production through water electrolysis is considered the next-generation technology capable of industrial-scale hydrogen production to achieve carbon neutrality. The core of constructing a water electrolyzer lies in designing the membrane electrode assembly (MEA) with optimal integration of the membrane, electrocatalysts, and gas diffusion layer. Among the two representative MEA fabrication methods, catalyst-coated substrates (CCS) and catalyst-coated membranes (CCM), CCM shows great promise due to its catalyst layer/membrane interface contact and scalability. The key factor in the CCM method is the effective application of the powdered catalyst onto the membrane. In this respect, the utilization of single-atom catalysts (SACs) has emerged as a noteworthy focus due to their unprecedented catalytic activity resulting from unique electronic/atomic configurations and high atomic utilization efficiency. Incorporating SACs into CCM–MEA has the potential to be a cutting-edge water electrolysis technology. However, it is still in its infancy due to the instability of the components (SACs, membranes, ionomers, supports) and degradation during the SACs–CCM–MEA fabrication and cell operation. Herein, we outline the representative fabrication method of MEA and provide a comprehensive analysis of SACs applicable to MEA. Then, we discuss the advantages of SACs–CCM–MEA and the challenges for industrial hydrogen production. Finally, this review concludes with future perspectives on the development of single-atom catalyst-coated membranes and the expected achievements.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 49-70"},"PeriodicalIF":0.0,"publicationDate":"2023-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00165b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519294","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Gas-phase errors in computational electrocatalysis: a review 计算电催化中的气相误差综述
EES catalysis Pub Date : 2023-09-29 DOI: 10.1039/D3EY00126A
Ricardo Urrego-Ortiz, Santiago Builes, Francesc Illas and Federico Calle-Vallejo
{"title":"Gas-phase errors in computational electrocatalysis: a review","authors":"Ricardo Urrego-Ortiz, Santiago Builes, Francesc Illas and Federico Calle-Vallejo","doi":"10.1039/D3EY00126A","DOIUrl":"10.1039/D3EY00126A","url":null,"abstract":"<p >Currently, computational models based on density functional theory (DFT) are intensively used for the analysis of electrocatalytic reactions and the design of enhanced catalysts. As the accuracy of these models is subjected to the quality of the input data, knowing the intrinsic limitations of DFT is crucial to improve computational predictions. A common pitfall of DFT is the estimation of the total energies of molecules, particularly those containing double and triple bonds. In this review, we show how gas-phase errors permeate thermodynamic and kinetic models of customary use in electrocatalysis, potentially compromising their predictiveness. First, we illustrate how these errors can be identified and provide a list of corrections for common molecules and functional groups. Subsequently, we explain how the errors spread from simple reaction energy calculations to adsorption energies, scaling relations, equilibrium potentials, overpotentials, and Sabatier-type activity plots. Finally, we list the remaining challenges toward an improved assessment of energetics at solid–gas–liquid interfaces.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 1","pages":" 157-179"},"PeriodicalIF":0.0,"publicationDate":"2023-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/ey/d3ey00126a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138519306","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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