Pub Date : 2025-10-16DOI: 10.1016/j.checat.2025.101546
Yan Wang, Wei Wang, Yanan Li, Haichuan He, Min Yu, Liqiang Wang, Junyan Wang, Liu Deng, Guipeng Yu, You-Nian Liu, Heinz-Bernhard Kraatz
Reducing an N=O group while maintaining the integrity of the labile N–O remains a serious challenge in nitro reduction. Here, we report a linker protonation strategy that provides control over the interactions between the catalyst and substrate, allowing the selective reduction of nitroaromatics to aromatic hydroxylamines in a photocatalytic hydrogenation reaction. Covalent organic frameworks (COFs) are ideal for this purpose and are used to control the electronic structure and the catalytic microenvironment, resulting in a 2-fold increase in the internal electric field and a more than 200-fold increase in shallow-charge-trapping lifetime. This improves the charge separation and proton transfer, enhancing the interactions between the COFs and nitroaromatics, resulting in a rapid quantitative conversion of nitrobenzene to N-phenylhydroxylamine, with a selectivity of >99%.
{"title":"Covalent organic frameworks with protonation control for selective photocatalytic nitroaromatic reduction","authors":"Yan Wang, Wei Wang, Yanan Li, Haichuan He, Min Yu, Liqiang Wang, Junyan Wang, Liu Deng, Guipeng Yu, You-Nian Liu, Heinz-Bernhard Kraatz","doi":"10.1016/j.checat.2025.101546","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101546","url":null,"abstract":"Reducing an N=O group while maintaining the integrity of the labile N–O remains a serious challenge in nitro reduction. Here, we report a linker protonation strategy that provides control over the interactions between the catalyst and substrate, allowing the selective reduction of nitroaromatics to aromatic hydroxylamines in a photocatalytic hydrogenation reaction. Covalent organic frameworks (COFs) are ideal for this purpose and are used to control the electronic structure and the catalytic microenvironment, resulting in a 2-fold increase in the internal electric field and a more than 200-fold increase in shallow-charge-trapping lifetime. This improves the charge separation and proton transfer, enhancing the interactions between the COFs and nitroaromatics, resulting in a rapid quantitative conversion of nitrobenzene to <em>N</em>-phenylhydroxylamine, with a selectivity of >99%.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"5 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145295428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-15DOI: 10.1016/j.checat.2025.101525
Zhuoyang Xie, Junhui Yan, Xiufang Zheng, Na Yang, Wei Ding, Li Li, Zidong Wei
Understanding and modeling the complex interplay between catalytic reactions and deactivation processes under operating conditions remains a major challenge. Using Fe–N–C oxygen reduction reaction catalysts as representative examples, we proposed a theoretical framework based on sequentially decoupling and recoupling Fe leaching with oxygen reduction to theoretically reveal a microscopic picture of degradation under operating conditions. We introduced a coupled mechanism network to isolate the role of each step in the leaching process. The quasi-steady-state approximation microkinetic modeling, bottom-up, reproduces experimentally observed first-order degradation kinetics and resolves their origins—that is, a competitive relationship between sluggish leaching rates and fast oxygen reduction turnover. We identified two strategies to stabilize the Fe sites: forming inner H-bonds and facilitating bridge-type O formation to stabilize leaching intermediates, suppressing Fe leaching and increasing activity and stability simultaneously. This work establishes a link between atomic-level fundamental mechanisms and electrocatalyst deactivation.
理解和模拟操作条件下催化反应和失活过程之间复杂的相互作用仍然是一个主要挑战。以Fe - n - c氧还原反应催化剂为代表，提出了一个基于铁浸出与氧还原顺序解耦和重耦的理论框架，从理论上揭示了操作条件下铁浸出与氧还原的微观降解图景。我们引入了一个耦合机制网络来隔离浸出过程中每个步骤的作用。自底向上的准稳态近似微动力学模型再现了实验观察到的一级降解动力学，并解决了它们的起源——即缓慢的浸出率和快速的氧还原周转率之间的竞争关系。我们确定了两种稳定Fe位点的策略：形成内部氢键和促进桥型O的形成以稳定浸出中间体，同时抑制Fe浸出并增加活性和稳定性。这项工作建立了原子水平的基本机制和电催化剂失活之间的联系。
{"title":"Kinetic analysis of Fe leaching and stability in Fe–N–C catalysts during oxygen reduction","authors":"Zhuoyang Xie, Junhui Yan, Xiufang Zheng, Na Yang, Wei Ding, Li Li, Zidong Wei","doi":"10.1016/j.checat.2025.101525","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101525","url":null,"abstract":"Understanding and modeling the complex interplay between catalytic reactions and deactivation processes under operating conditions remains a major challenge. Using Fe–N–C oxygen reduction reaction catalysts as representative examples, we proposed a theoretical framework based on sequentially decoupling and recoupling Fe leaching with oxygen reduction to theoretically reveal a microscopic picture of degradation under operating conditions. We introduced a coupled mechanism network to isolate the role of each step in the leaching process. The quasi-steady-state approximation microkinetic modeling, bottom-up, reproduces experimentally observed first-order degradation kinetics and resolves their origins—that is, a competitive relationship between sluggish leaching rates and fast oxygen reduction turnover. We identified two strategies to stabilize the Fe sites: forming inner H-bonds and facilitating bridge-type O formation to stabilize leaching intermediates, suppressing Fe leaching and increasing activity and stability simultaneously. This work establishes a link between atomic-level fundamental mechanisms and electrocatalyst deactivation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"53 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145289278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Palladium (Pd) nanocatalyst-loaded covalent organic framework (COF) membranes emerge as a promising platform for efficient water decontamination. Here, we propose the concept of affinity-induced confinement, which involves using COF membranes (TpTGCl) for selective Pd capture from simulated acid wastewater. Size regulation of the Pd nanocatalyst within COF membranes was achieved. The resulting catalytic membranes loaded with Pd nanoclusters (PdNC-TpTGCl) demonstrate exceptional sieving of organic pollutants and high catalytic activity, achieving a remarkable 99.7% conversion of 4-nitrophenol to 4-aminophenol. This performance is attributed to the uniform distribution of ultrafine nanoclusters (2.4 nm) and the nanofluidic confinement effect of COF channels. Molecular simulations and calculations reveal that the ultra-fast reaction rate of 4-NP is facilitated by the Eley-Rideal mechanism when passing through the PdNC-TpTGCl membrane. Overall, our methodology for multifunctional, recyclable, PdNC-loaded COF membranes is applicable to the development of efficient coupled sieving and catalysis membranes for a variety of applications.
{"title":"Affinity-induced upcycling of palladium nanoclusters in COF membranes for catalytic water treatment","authors":"Shaochong Cao, Makenna Parkinson, Junyong Zhu, Zihao Zhai, Yatao Zhang, Tao He, Menachem Elimelech","doi":"10.1016/j.checat.2025.101524","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101524","url":null,"abstract":"Palladium (Pd) nanocatalyst-loaded covalent organic framework (COF) membranes emerge as a promising platform for efficient water decontamination. Here, we propose the concept of affinity-induced confinement, which involves using COF membranes (TpTG<sub>Cl</sub>) for selective Pd capture from simulated acid wastewater. Size regulation of the Pd nanocatalyst within COF membranes was achieved. The resulting catalytic membranes loaded with Pd nanoclusters (Pd<sub>NC</sub>-TpTG<sub>Cl</sub>) demonstrate exceptional sieving of organic pollutants and high catalytic activity, achieving a remarkable 99.7% conversion of 4-nitrophenol to 4-aminophenol. This performance is attributed to the uniform distribution of ultrafine nanoclusters (2.4 nm) and the nanofluidic confinement effect of COF channels. Molecular simulations and calculations reveal that the ultra-fast reaction rate of 4-NP is facilitated by the Eley-Rideal mechanism when passing through the Pd<sub>NC</sub>-TpTG<sub>Cl</sub> membrane. Overall, our methodology for multifunctional, recyclable, Pd<sub>NC</sub>-loaded COF membranes is applicable to the development of efficient coupled sieving and catalysis membranes for a variety of applications.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"12 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145283768","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-07DOI: 10.1016/j.checat.2025.101519
Thu N. Ton, Haochen Zhang, Paul H. Oyala, Gang San Lee, Karthish Manthiram
The electrochemical carboxylation of aldehydes with carbon dioxide (CO2) is a sustainable strategy to synthesize industrially relevant ɑ-hydroxycarboxylic acids under mild conditions while avoiding toxic sodium cyanide. However, this reaction remains hindered by low activity and selectivity due to a limited understanding of the reaction mechanism. In this work, we present a mechanistic study of electrochemical benzaldehyde carboxylation. In situ electron paramagnetic resonance spectroscopy demonstrated that the reaction occurs via a ketyl radical intermediate generated from the one-electron reduction of benzaldehyde. Electrochemical kinetic analysis suggested the rate-determining step to be the subsequent coupling of the surface-bound ketyl radical with CO2. Finally, our investigation revealed that the optimal reaction rate and selectivity were achieved in the presence of Lewis acidic magnesium cations, resulting in the highest Faradaic efficiency of 79% and a partial current density of 12.9 mA/cm2.
{"title":"Electrochemical benzaldehyde carboxylation for sustainable mandelic acid synthesis via radical intermediates","authors":"Thu N. Ton, Haochen Zhang, Paul H. Oyala, Gang San Lee, Karthish Manthiram","doi":"10.1016/j.checat.2025.101519","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101519","url":null,"abstract":"The electrochemical carboxylation of aldehydes with carbon dioxide (CO<sub>2</sub>) is a sustainable strategy to synthesize industrially relevant <em>ɑ</em>-hydroxycarboxylic acids under mild conditions while avoiding toxic sodium cyanide. However, this reaction remains hindered by low activity and selectivity due to a limited understanding of the reaction mechanism. In this work, we present a mechanistic study of electrochemical benzaldehyde carboxylation. <em>In situ</em> electron paramagnetic resonance spectroscopy demonstrated that the reaction occurs via a ketyl radical intermediate generated from the one-electron reduction of benzaldehyde. Electrochemical kinetic analysis suggested the rate-determining step to be the subsequent coupling of the surface-bound ketyl radical with CO<sub>2</sub>. Finally, our investigation revealed that the optimal reaction rate and selectivity were achieved in the presence of Lewis acidic magnesium cations, resulting in the highest Faradaic efficiency of 79% and a partial current density of 12.9 mA/cm<sup>2</sup>.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"7 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Iron-based compounds transform in situ into iron (oxyhydr)oxides (FeOxHy) during the alkaline oxygen evolution reaction (OER), serving as active species but suffering from aggregation, poor conductivity, and Fe leaching. To address these limitations, we employ the heterobimetallic rare-earth transition-metal-based Laves-phase CeFe2 as an OER precatalyst. The robust chemical bonding, ordered atomic arrangement, and inherent oxophilic nature of Ce in the structure drive in situ surface reconstruction of fully oxidized CeFe2 to a heterostructure composed of α-FeOOH nanodomains uniformly confined within CeO2. Comprehensive analyses, including quasi-in situ Raman and X-ray absorption spectroscopy, scanning transmission electron microscopy, and theoretical calculations, confirm that non-leaching CeO2 prevents Fe dissolution, suppresses α-FeOOH aggregation, and optimizes its electronic structure and rate-determining step. Moreover, the remaining bulk CeFe2 phase improves charge transfer, collectively enabling the CeFe2-based system to significantly outperform directly synthesized FeOxHy references and rival the benchmark NiFeOxHy in OER.
{"title":"Non-leaching cerium oxide evolved from Laves phase enables iron-retentive oxygen evolution","authors":"Ziliang Chen, Hongyuan Yang, Ruotao Yang, Tamanna Manjur Ahamad, Guoliang Dai, Ingo Zebger, Matthias Driess, Prashanth W. Menezes","doi":"10.1016/j.checat.2025.101518","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101518","url":null,"abstract":"Iron-based compounds transform <em>in situ</em> into iron (oxyhydr)oxides (FeO<sub><em>x</em></sub>H<sub><em>y</em></sub>) during the alkaline oxygen evolution reaction (OER), serving as active species but suffering from aggregation, poor conductivity, and Fe leaching. To address these limitations, we employ the heterobimetallic rare-earth transition-metal-based Laves-phase CeFe<sub>2</sub> as an OER precatalyst. The robust chemical bonding, ordered atomic arrangement, and inherent oxophilic nature of Ce in the structure drive <em>in situ</em> surface reconstruction of fully oxidized CeFe<sub>2</sub> to a heterostructure composed of α-FeOOH nanodomains uniformly confined within CeO<sub>2</sub>. Comprehensive analyses, including quasi-<em>in situ</em> Raman and X-ray absorption spectroscopy, scanning transmission electron microscopy, and theoretical calculations, confirm that non-leaching CeO<sub>2</sub> prevents Fe dissolution, suppresses α-FeOOH aggregation, and optimizes its electronic structure and rate-determining step. Moreover, the remaining bulk CeFe<sub>2</sub> phase improves charge transfer, collectively enabling the CeFe<sub>2</sub>-based system to significantly outperform directly synthesized FeO<sub><em>x</em></sub>H<sub><em>y</em></sub> references and rival the benchmark NiFeO<sub><em>x</em></sub>H<sub><em>y</em></sub> in OER.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"35 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241622","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-10-07DOI: 10.1016/j.checat.2025.101544
Xinyang Gao, Chenyuan Zhu, Liming Zhang
Tandem electrocatalysis enhances small-molecule conversion efficiency and selectivity by modulating reaction intermediates. This review examines key intermediates in systems such as CO2 reduction, nitrate reduction, and C–N coupling. The critical roles of ∗CO, H, and NO2− intermediates are discussed. Advances in catalyst design, including dual-metal sites, interface modifications, and dynamic restructuring, are highlighted for their effects on intermediate adsorption and activation. Challenges remain in controlling intermediate pathways to improve selectivity and activity. This overview provides insights into rational catalyst-design strategies for sustainable energy and chemical production, emphasizing the importance of intermediate regulation in tandem electrocatalytic processes.
{"title":"Intermediate regulation strategies in tandem electrocatalysis for small-molecule conversion","authors":"Xinyang Gao, Chenyuan Zhu, Liming Zhang","doi":"10.1016/j.checat.2025.101544","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101544","url":null,"abstract":"Tandem electrocatalysis enhances small-molecule conversion efficiency and selectivity by modulating reaction intermediates. This review examines key intermediates in systems such as CO<sub>2</sub> reduction, nitrate reduction, and C–N coupling. The critical roles of ∗CO, H, and NO<sub>2</sub><sup>−</sup> intermediates are discussed. Advances in catalyst design, including dual-metal sites, interface modifications, and dynamic restructuring, are highlighted for their effects on intermediate adsorption and activation. Challenges remain in controlling intermediate pathways to improve selectivity and activity. This overview provides insights into rational catalyst-design strategies for sustainable energy and chemical production, emphasizing the importance of intermediate regulation in tandem electrocatalytic processes.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"13 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241621","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-29DOI: 10.1016/j.checat.2025.101517
Wen Zhou, Shan Wang, Mathias Dimde, Kai Ludwig, Henrik Karring, Changzhu Wu
Chemoenzymatic cascade, integrating chemical catalysis and biocatalysis within a single system, presents transformative opportunities in chemical bioconversion. However, the implementation of such catalytic systems remains challenging due to inherent incompatibilities between chemical and enzymatic processes. To address that, we developed a biocompatible approach that combines polymeric micelles with living cells to achieve a recyclable photoenzymatic cascade. In this process, the charged micelles encapsulating photocatalysts are attached to the surface of benzaldehyde lyase-expressing Escherichia coli (E. coli) cells. Notably, the coated E. coli cells not only retained their intrinsic enzymatic activity but also enabled an efficient one-pot photoenzymatic cascade. Furthermore, the micelle-coated cells retained over 83% of their original activity after five catalytic cycles. Consequently, our approach offers a polymeric micellar platform for achieving a recyclable photoenzymatic cascade, with the potential to be extended to other chemoenzymatic cascades, thereby providing a promising strategy for efficient industrial synthesis.
{"title":"Integrating micelle catalysts with living cells for recyclable photoenzymatic cascades","authors":"Wen Zhou, Shan Wang, Mathias Dimde, Kai Ludwig, Henrik Karring, Changzhu Wu","doi":"10.1016/j.checat.2025.101517","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101517","url":null,"abstract":"Chemoenzymatic cascade, integrating chemical catalysis and biocatalysis within a single system, presents transformative opportunities in chemical bioconversion. However, the implementation of such catalytic systems remains challenging due to inherent incompatibilities between chemical and enzymatic processes. To address that, we developed a biocompatible approach that combines polymeric micelles with living cells to achieve a recyclable photoenzymatic cascade. In this process, the charged micelles encapsulating photocatalysts are attached to the surface of benzaldehyde lyase-expressing <em>Escherichia coli</em> (<em>E. coli</em>) cells. Notably, the coated <em>E. coli</em> cells not only retained their intrinsic enzymatic activity but also enabled an efficient one-pot photoenzymatic cascade. Furthermore, the micelle-coated cells retained over 83% of their original activity after five catalytic cycles. Consequently, our approach offers a polymeric micellar platform for achieving a recyclable photoenzymatic cascade, with the potential to be extended to other chemoenzymatic cascades, thereby providing a promising strategy for efficient industrial synthesis.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"17 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183392","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-26DOI: 10.1016/j.checat.2025.101523
Sallye R. Gathmann, Seongjoo Jung, Paul J. Dauenhauer
Microkinetic models are useful tools for screening catalytic materials; however, errors in their input parameters can lead to significant uncertainty in model predictions of catalyst performance. Here, we investigate the impact of linear scaling and Brønsted-Evans-Polanyi relation parametric uncertainty on microkinetic predictions of programmable-catalyst performance. Two case studies are considered: a generic A-to-B prototype reaction and the oxygen evolution reaction (OER). The results show that error-unaware models can accurately predict trends and, for the prototype reaction, values of optimal waveform parameters. The specific model parameters driving output uncertainty are identified via variance-based global sensitivity analysis. However, predictions of dynamic rate enhancement can decrease when uncertainty is propagated into the models. In both cases, we identify operating conditions where the programmable catalyst achieves a rate enhancement of at least one order of magnitude despite parametric uncertainty in the model, supporting programmable catalysis as a viable strategy for exceeding the Sabatier limit.
{"title":"Catalytic resonance theory for parametric uncertainty of programmable catalysis","authors":"Sallye R. Gathmann, Seongjoo Jung, Paul J. Dauenhauer","doi":"10.1016/j.checat.2025.101523","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101523","url":null,"abstract":"Microkinetic models are useful tools for screening catalytic materials; however, errors in their input parameters can lead to significant uncertainty in model predictions of catalyst performance. Here, we investigate the impact of linear scaling and Brønsted-Evans-Polanyi relation parametric uncertainty on microkinetic predictions of programmable-catalyst performance. Two case studies are considered: a generic A-to-B prototype reaction and the oxygen evolution reaction (OER). The results show that error-unaware models can accurately predict trends and, for the prototype reaction, values of optimal waveform parameters. The specific model parameters driving output uncertainty are identified via variance-based global sensitivity analysis. However, predictions of dynamic rate enhancement can decrease when uncertainty is propagated into the models. In both cases, we identify operating conditions where the programmable catalyst achieves a rate enhancement of at least one order of magnitude despite parametric uncertainty in the model, supporting programmable catalysis as a viable strategy for exceeding the Sabatier limit.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"15 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153758","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-24DOI: 10.1016/j.checat.2025.101516
Ao Yu, Yang Yang
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Ao Yu earned his PhD from the Huazhong University of Science and Technology. He joined Prof. Yang’s group as a postdoctoral researcher supported by the Preeminent Postdoctoral Program (P3) in February 2023. His research interests focus on electrochemical energy storage and conversion, especially in the fields of oxygen reduction catalysts, batteries, and molten salt CO2 capture and conversion.
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Yang Yang is a professor at the University of Central Florida. His research focuses on the surface and interface electrochemistry of energy materials and devices, materials science, nanomanufacturing, electrochemical engineering, and nanoscience technology. His homepage is http://www.yangyanglab.com.
{"title":"Design of electrolyzers for sustainable H2O2 electrosynthesis","authors":"Ao Yu, Yang Yang","doi":"10.1016/j.checat.2025.101516","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101516","url":null,"abstract":"<span><figure><span><img alt=\"\" height=\"341\" src=\"https://ars.els-cdn.com/content/image/1-s2.0-S2667109325002544-fx2.jpg\"/><ol><li><span><span>Download: <span>Download high-res image (293KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span>Ao Yu earned his PhD from the Huazhong University of Science and Technology. He joined Prof. Yang’s group as a postdoctoral researcher supported by the Preeminent Postdoctoral Program (P3) in February 2023. His research interests focus on electrochemical energy storage and conversion, especially in the fields of oxygen reduction catalysts, batteries, and molten salt CO<sub>2</sub> capture and conversion.<span><figure><span><img alt=\"\" height=\"341\" src=\"https://ars.els-cdn.com/content/image/1-s2.0-S2667109325002544-fx3.jpg\"/><ol><li><span><span>Download: <span>Download high-res image (298KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span>Yang Yang is a professor at the University of Central Florida. His research focuses on the surface and interface electrochemistry of energy materials and devices, materials science, nanomanufacturing, electrochemical engineering, and nanoscience technology. His homepage is <span><span>http://www.yangyanglab.com</span><svg aria-label=\"Opens in new window\" focusable=\"false\" height=\"20\" viewbox=\"0 0 8 8\"><path d=\"M1.12949 2.1072V1H7V6.85795H5.89111V2.90281L0.784057 8L0 7.21635L5.11902 2.1072H1.12949Z\"></path></svg></span>.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"38 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145127980","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-23DOI: 10.1016/j.checat.2025.101521
Xing Yuan, Wenzhe Si, Xiao Zhu, Bin Zhou, Yue Peng, Junhua Li
Platinum (Pt) atomic single-layer (ASL) can trigger synergistic effects between metal atoms and surface moieties of supports, which governs its catalytic activity and product selectivity. The electronic metal-support interaction determines not only the local coordination environment in shaping the stability and reactivity of Pt on support, but also the covalency of Pt–O and electron transfer properties. Here, we reveal the impact of different anchoring mechanisms between Pt ASL and supports on catalytic activity and product selectivity of NH3 oxidation. The Pt ASL consumes more low-coordination terminal hydroxyls on Al2O3, and the lower coordination number leads to the stronger electron transfer between Pt ASL and TiO2. The imino group acts as the key intermediate on Pt/TiO2 resulting in higher NH3 conversion but lower N2 selectivity, whereas the amino group plays a dominant role on Pt/Al2O3 leading to slightly lower NH3 conversion but higher N2 selectivity because of rapid NH3∗ dehydrogenation.
{"title":"Hydroxyl anchoring and electron transfer behaviors of atomic single-layer Pt in NH3 oxidation","authors":"Xing Yuan, Wenzhe Si, Xiao Zhu, Bin Zhou, Yue Peng, Junhua Li","doi":"10.1016/j.checat.2025.101521","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101521","url":null,"abstract":"Platinum (Pt) atomic single-layer (ASL) can trigger synergistic effects between metal atoms and surface moieties of supports, which governs its catalytic activity and product selectivity. The electronic metal-support interaction determines not only the local coordination environment in shaping the stability and reactivity of Pt on support, but also the covalency of Pt–<em>O</em> and electron transfer properties. Here, we reveal the impact of different anchoring mechanisms between Pt ASL and supports on catalytic activity and product selectivity of NH<sub>3</sub> oxidation. The Pt ASL consumes more low-coordination terminal hydroxyls on Al<sub>2</sub>O<sub>3</sub>, and the lower coordination number leads to the stronger electron transfer between Pt ASL and TiO<sub>2</sub>. The imino group acts as the key intermediate on Pt/TiO<sub>2</sub> resulting in higher NH<sub>3</sub> conversion but lower N<sub>2</sub> selectivity, whereas the amino group plays a dominant role on Pt/Al<sub>2</sub>O<sub>3</sub> leading to slightly lower NH<sub>3</sub> conversion but higher N<sub>2</sub> selectivity because of rapid NH<sub>3</sub>∗ dehydrogenation.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"19 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145116727","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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