EES catalysis最新文献_第2页

Vibrationally excited molecule–metal surface reactions in heterogeneous and plasma catalysis: going beyond the Fridman–Macheret α model 非均相和等离子体催化中振动激发的分子-金属表面反应：超越Fridman-Macheret α模型。

EES catalysis Pub Date : 2025-04-22 DOI: 10.1039/D5EY00062A

Nick Gerrits and Annemie Bogaerts

{"title":"Vibrationally excited molecule–metal surface reactions in heterogeneous and plasma catalysis: going beyond the Fridman–Macheret α model","authors":"Nick Gerrits and Annemie Bogaerts","doi":"10.1039/D5EY00062A","DOIUrl":"10.1039/D5EY00062A","url":null,"abstract":"Vibrational excitation of reactants plays an important role in heterogeneous and plasma catalysis by increasing the reactivity of various rate-controlling steps. Therefore, state-of-the-art microkinetic models attempt to include this effect by modelling the change in reaction rate with the Fridman–Macheret α approach. Although this approach is ubiquitous in simulations of plasma catalysis, it is not well established how accurate it is. In this work, we evaluate the Fridman–Macheret α approach by comparing it to vibrational efficacies obtained with molecular dynamics simulations. Unfortunately, the agreement is extremely poor (R2 = −0.35), raising questions about the suitability of using this method in describing vibrationally excited dissociative chemisorption on metal surfaces, as is currently the norm in plasma catalysis. Furthermore, the approach lacks vibrational mode specificity. Instead, we propose an alternative model at comparable computational cost, which is fitted to theoretical vibrational efficacies obtained with molecular dynamics. Our model uses (1) the barrier height to dissociative chemisorption, (2) an indication of how “late” the barrier is, and (3) the overlap of vibrational modes and the reaction coordinate at the barrier. These three features lead to a considerable qualitative and quantitative (R2 = 0.52) improvement over the Fridman–Macheret α approach. Therefore, we advise to make use of our new model, since it can be readily plugged into existing microkinetic models for heterogeneous and plasma catalysis.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 733-742"},"PeriodicalIF":0.0,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12077265/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144095892","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

Constructing four-in-one catalysts to realize ultralow voltage hydrogen production at ampere-level current densities† 构建四合一催化剂，实现安培级电流密度下的超低电压制氢

EES catalysis Pub Date : 2025-04-18 DOI: 10.1039/D5EY00117J

Minghui Xing, Mengting Han, Guoqing Xu, Zhiping Liu, Qinglan Zhao, Minhua Shao, Jimmy Yun, Peng Wang and Dapeng Cao

{"title":"Constructing four-in-one catalysts to realize ultralow voltage hydrogen production at ampere-level current densities†","authors":"Minghui Xing, Mengting Han, Guoqing Xu, Zhiping Liu, Qinglan Zhao, Minhua Shao, Jimmy Yun, Peng Wang and Dapeng Cao","doi":"10.1039/D5EY00117J","DOIUrl":"https://doi.org/10.1039/D5EY00117J","url":null,"abstract":"An anion exchange membrane water electrolyzer (AEMWE) is emerging as key technology for hydrogen production. However, its widespread application requires further reduction of cost and improvement of efficiencies. Here, we synthesize a four-in-one catalyst (VSA-CoNx) to achieve high-efficiency coupling hydrogen production by combining with the hydrazine oxidation reaction (HzOR) and the urea oxidation reaction (UOR). The as-synthesized VSA-CoNx exhibits excellent performance in all the four reactions of HzOR, UOR and hydrogen/oxygen evolution reactions (HER/OER). The HER–HzOR coupling system only requires an ultra-low voltage of 0.21 V to deliver an ampere-level current density (1 A cm−2), while the conventional HER–OER AEMWE needs nearly an input of 1.88 V. Remarkably, this HER–HzOR coupling system largely reduces the energy expenditure of the AEMWE by approximately 90%, which hits a record in the low energy cost for all water electrolysis systems known to date. Given the energy consumption of the traditional AEMWE of approximately 4.56 kW h Nm−3 of H2 at a current density of 1 A cm−2, the HER–HzOR AEM electrolyzer only requires 0.51 kW h Nm−3 of H2. This HER–HzOR coupling system not only significantly lowers the energy expenditure of large-scale H2 production but also addresses the hydrazine-associated environmental pollution.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 832-842"},"PeriodicalIF":0.0,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00117j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144536808","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

Enhanced activity and stability of polymeric carbon nitride photoanodes by yttrium incorporation† 钇掺入†增强聚合物氮化碳光阳极的活性和稳定性

EES catalysis Pub Date : 2025-04-17 DOI: 10.1039/D5EY00064E

Sanjit Mondal, Ayelet Tashakory, Gabriel Mark, Shmuel Barzilai, Angus Pedersen, Michael Volokh, Josep Albero, Hermenegildo García and Menny Shalom

{"title":"Enhanced activity and stability of polymeric carbon nitride photoanodes by yttrium incorporation†","authors":"Sanjit Mondal, Ayelet Tashakory, Gabriel Mark, Shmuel Barzilai, Angus Pedersen, Michael Volokh, Josep Albero, Hermenegildo García and Menny Shalom","doi":"10.1039/D5EY00064E","DOIUrl":"https://doi.org/10.1039/D5EY00064E","url":null,"abstract":"Polymeric carbon nitride materials (CNs) show promising potential as photoanodes in water-splitting photoelectrochemical cells. However, poor catalytic activity at the electrode–water interface limits their performance and longevity, resulting in low photoactivity and unwanted self-oxidation. Here, we demonstrate a high-performance photoanode based on polymeric carbon nitride doped with yttrium clusters, achieving enhanced activity and stability with high faradaic efficiency for water oxidation. Incorporating yttrium clusters enhances light harvesting, electronic conductivity, charge separation, and hole extraction kinetics, enabling efficient water oxidation. Furthermore, the strong interaction between yttrium and the CN's nitrogen groups guides the formation of yttrium-rich one-dimensional tubular structures that interconnect two-dimensional CN sheets. The optimized photoanode delivers a photocurrent density of 275 ± 10 μA cm−2 with 90% faradaic efficiency for oxygen evolution, demonstrates stable performance for up to 10 hours, and achieves external quantum efficiencies of up to 14% in an alkaline medium.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 800-810"},"PeriodicalIF":0.0,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00064e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144536805","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

Direct conversion of CO2 to aromatics based on the coupling strategy and multi-functional catalysis 基于耦合策略和多功能催化的CO2直接转化为芳烃

EES catalysis Pub Date : 2025-04-09 DOI: 10.1039/D5EY00052A

Chang Liu, Yangdong Wang, Lin Zhang, Junjie Su, Su Liu, Haibo Zhou, Wenqian Jiao and Zaiku Xie

{"title":"Direct conversion of CO2 to aromatics based on the coupling strategy and multi-functional catalysis","authors":"Chang Liu, Yangdong Wang, Lin Zhang, Junjie Su, Su Liu, Haibo Zhou, Wenqian Jiao and Zaiku Xie","doi":"10.1039/D5EY00052A","DOIUrl":"https://doi.org/10.1039/D5EY00052A","url":null,"abstract":"As fundamental chemicals and building blocks for the modern chemical industry, aromatics possess a huge market demand. The direct and atom-economic conversion of CO2 to aromatics holds the potential to diminish the reliance on petroleum resources and provides a viable approach towards a net-zero chemical industry. The key lies in the implementation of the highly efficient coupling catalysis strategy and utilization of multi-functional catalysts. In this review, recent advances in the direct conversion of CO2 to aromatics via the methanol-mediated pathway and the modified Fischer–Tropsch synthesis route are comprehensively discussed, including an in-depth analysis of the tandem reaction mechanism and bifunctional catalysts, which consist of metal-based materials (including metals, metal oxides, or metal carbides) and zeolites. Furthermore, several novel catalytic pathways, involving coupling CO2 conversion with reactions such as CO hydrogenation, aromatic alkylation, or alkane aromatization, are also elaborated. Subsequently, the coupling effect of multi-functional catalysis, as well as the influence of the proximity between catalytic components, is explored. Moreover, the revealing and construction of the spatial pathway for tandem reactions, which enable the spatio-temporal coupling of multi-functional catalytic systems, are addressed. The challenges and potential directions for the further development of the direct CO2-to-aromatics conversion technology are finally proposed.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 621-643"},"PeriodicalIF":0.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00052a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144536768","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

Plasma catalysis: what is needed to create synergy? 等离子体催化：需要什么来产生协同作用？

EES catalysis Pub Date : 2025-04-02 DOI: 10.1039/D5EY00027K

Joran Van Turnhout, Kevin Rouwenhorst, Leon Lefferts and Annemie Bogaerts

引用次数: 0

Correction: Single atom catalysts for water electrolysis: from catalyst-coated substrate to catalyst-coated membrane 修正：水电解用单原子催化剂：从被催化剂包覆的底物到被催化剂包覆的膜

EES catalysis Pub Date : 2025-04-01 DOI: 10.1039/D5EY90009C

Sol A Lee, Sang Eon Jun, Sun Hwa Park, Ki Chang Kwon, Jong Hun Kang, Min Sang Kwon and Ho Won Jang

引用次数: 0

Two-step tandem electrochemical conversion of oxalic acid and nitrate to glycine† 草酸和硝酸盐两步串联电化学转化为甘氨酸。

EES catalysis Pub Date : 2025-03-31 DOI: 10.1039/D5EY00016E

Yuan-Zi Xu, Daniel F. Abbott, Lok Nga Poon and Victor Mougel

{"title":"Two-step tandem electrochemical conversion of oxalic acid and nitrate to glycine†","authors":"Yuan-Zi Xu, Daniel F. Abbott, Lok Nga Poon and Victor Mougel","doi":"10.1039/D5EY00016E","DOIUrl":"10.1039/D5EY00016E","url":null,"abstract":"This study presents a facile tandem strategy for improving the efficiency of glycine electrosynthesis from oxalic acid and nitrate. In this tandem electrocatalytic process, oxalic acid is first reduced to glyoxylic acid, while nitrate is reduced to hydroxylamine. Subsequent coupling of these two precursors results in the formation of a C–N bond, producing the intermediate glyoxylic acid oxime, which is further reduced in situ to glycine. Here we show, using only a simple Pb foil electrode, which maximizes the yield of the first step of the transformation (i.e. the reduction of oxalic acid to glyoxylic acid) prior to the coupling step allows for an unprecedented selectivity and conversion for glycine electrosynthesis to be achieved. Overall, a maximum glycine faradaic efficiency (FE) of 59% is achieved at −300 mA cm−2 and a high glycine partial current density of −232 mA cm−2 and a glycine production rate of 0.82 mmol h−1 cm−2 are attained at −400 mA cm−2, thereby paving the way for an energy and economically efficient electrochemical synthesis of glycine.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 783-789"},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11973474/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144051860","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

Breaking the selectivity-activity seesaw in ethane oxidative dehydrogenation via the synergetic effects of doping and electrochemical activation† 通过掺杂和电化学活化的协同作用打破乙烷氧化脱氢过程的选择性-活性跷跷板

EES catalysis Pub Date : 2025-03-28 DOI: 10.1039/D5EY00012B

Xiang Sun, Benchi Chen, Heejae Yang, Mengzhen Zhou, Nian Zhang, Yunkyung Kim, Wonyoung Lee, Jeong Woo Han, Zhang Lin and Yan Chen

{"title":"Breaking the selectivity-activity seesaw in ethane oxidative dehydrogenation via the synergetic effects of doping and electrochemical activation†","authors":"Xiang Sun, Benchi Chen, Heejae Yang, Mengzhen Zhou, Nian Zhang, Yunkyung Kim, Wonyoung Lee, Jeong Woo Han, Zhang Lin and Yan Chen","doi":"10.1039/D5EY00012B","DOIUrl":"https://doi.org/10.1039/D5EY00012B","url":null,"abstract":"The oxidative dehydrogenation (ODH) of alkanes using a solid oxide electrolysis cell (SOEC) has attracted worldwide attention as an efficient method for producing ethylene. Nevertheless, it remains challenging to achieve both a high alkane conversion rate and high ethylene selectivity. In this work, we demonstrate that the combination of doping and electrochemical activation can break this activity–selectivity seesaw and achieve a high ethylene yield. Using Sr2Ti0.8(Co1.2−xFex)O6−δ with different dopants as model electrodes, we show that increasing the Fe content efficiently lowers the oxygen activity by weakening metal–oxygen covalency, downshifting O 2p-band relative to the Fermi level, and increasing the oxygen vacancy formation energy. Such changes result in a lower ethane conversion rate but higher ethylene selectivity for Sr2Ti0.8Fe1.2O6−δ (STF) compared to electrodes with higher Co content. By increasing the applied potential, we can effectively increase the conversion rate of ethane without sacrificing too much ethylene selectivity. Ultimately, the SOEC with STF anode achieves an ethylene yield of up to 71% at 800 °C at 1.2 V with CO2 as the oxidant on the cathode side, which is among the highest documented. The insights gained from this study knowledge can guide the rational design of high-temperature electrochemical devices for other small molecule conversion reactions.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 790-799"},"PeriodicalIF":0.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00012b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144536804","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

Two-step polymerization for tailored donor–acceptor interactions driving efficient hydrogen evolution in visible-light photocatalysts† 两步聚合在可见光催化剂中驱动高效析氢的施主-受体相互作用

EES catalysis Pub Date : 2025-03-28 DOI: 10.1039/D5EY00035A

Wooteak Jung, Sanghyeok An, Gayoung Ham, Chanhyeok Kim, Soyeon Lee, Jiwoong Yang, Dae Sung Chung, Hyojung Cha and Taiho Park

{"title":"Two-step polymerization for tailored donor–acceptor interactions driving efficient hydrogen evolution in visible-light photocatalysts†","authors":"Wooteak Jung, Sanghyeok An, Gayoung Ham, Chanhyeok Kim, Soyeon Lee, Jiwoong Yang, Dae Sung Chung, Hyojung Cha and Taiho Park","doi":"10.1039/D5EY00035A","DOIUrl":"https://doi.org/10.1039/D5EY00035A","url":null,"abstract":"The development of materials for organic solar cells has made significant strides through the strategic combination of diverse donor structures with acceptor units in polymer backbones. In contrast, semiconducting polymers for photocatalytic hydrogen evolution have primarily focused on acceptor moieties, with limited exploration of donor contributions, primarily owing to the emphasis on designing active sites for proton reduction in inorganic catalysts. To investigate the impact of highly electron-donating moieties on photocatalytic performance, we designed and synthesized benzothiadiazole (BT)-based polymers with randomly incorporated benzodithiophene (BDT) and fluorene units via a streamlined one-pot Stille–Suzuki two-step polymerization. Comprehensive molecular characterization and optical spectroscopic analyses confirmed the successful synthesis of the target polymers. Photocatalytic hydrogen evolution studies, supported by photophysical and spectroscopic investigations, demonstrated that optimizing the proportion of BDT units in the polymer backbone enhances hydrogen evolution rates significantly. Additionally, comparative analyses further highlighted the distinct differences in the photocatalytic efficiency between the BDT and fluorene donor units, providing critical insights into their functional roles. This work underscores the potential of advancing polymer photocatalysts by fine-tuning donor–acceptor interactions through optimization of donor moiety composition, offering a robust framework for achieving superior photocatalytic performance.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 775-782"},"PeriodicalIF":0.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00035a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144536803","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

Identification of catalyst optimization trends for electrocatalytic CO(2) reduction to ethylene† 电催化CO(2)还原乙烯催化剂优化趋势的确定

EES catalysis Pub Date : 2025-03-27 DOI: 10.1039/D4EY00287C

Stefan J. Raaijman, Maarten P. Schellekens, Yoon Jun Son, Marc T. M. Koper and Paul J. Corbett

{"title":"Identification of catalyst optimization trends for electrocatalytic CO(2) reduction to ethylene†","authors":"Stefan J. Raaijman, Maarten P. Schellekens, Yoon Jun Son, Marc T. M. Koper and Paul J. Corbett","doi":"10.1039/D4EY00287C","DOIUrl":"https://doi.org/10.1039/D4EY00287C","url":null,"abstract":"In this perspective we analyze copper and copper-based electrocatalysts with high ethylene selectivities from the literature to identify global catalyst formulation trends that allow for making catalysts with improved ethylene performance for industrial application. From our analysis, we identified six trends that can aid researchers in creating novel, high selectivity electrocatalysts for the electroreduction of CO(2) to ethylene. These trends were as follows. (i) Tandem-type and (ii) supported-type catalysts perform relatively more poorly than other types of systems. Engineering the nanoenvironment through implementing nanoconfining morphologies (iii) or via the addition of polymeric additives (iv) brings about significant C2H4 selectivity enhancements. (v) Catalyst heterogeneity is an important driver for improving C2H4 selectivity. (vi) Both CO2 and CO can serve as feedstock with little impact on maximum achievable C2H4 selectivity. As we identified during our study that the field lacks reproducibility of catalyst performance and independent reproduction of results, we propose several strategies on how to improve. Finally, we discuss changes that authors can implement to improve the industrial relevancy of their work.","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 3","pages":" 386-406"},"PeriodicalIF":0.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d4ey00287c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143925352","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