Chem Catalysis最新文献

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Integrating micelle catalysts with living cells for recyclable photoenzymatic cascades 整合胶束催化剂与活细胞的可回收光酶级联
IF 9.4
Chem Catalysis Pub Date : 2025-09-29 DOI: 10.1016/j.checat.2025.101517
Wen Zhou, Shan Wang, Mathias Dimde, Kai Ludwig, Henrik Karring, Changzhu Wu
{"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}
引用次数: 0
Catalytic resonance theory for parametric uncertainty of programmable catalysis 可编程催化参数不确定的催化共振理论
IF 9.4
Chem Catalysis Pub Date : 2025-09-26 DOI: 10.1016/j.checat.2025.101523
Sallye R. Gathmann, Seongjoo Jung, Paul J. Dauenhauer
{"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}
引用次数: 0
Design of electrolyzers for sustainable H2O2 electrosynthesis 可持续H2O2电合成电解槽设计
IF 9.4
Chem Catalysis Pub Date : 2025-09-24 DOI: 10.1016/j.checat.2025.101516
Ao Yu, Yang Yang
{"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}
引用次数: 0
Hydroxyl anchoring and electron transfer behaviors of atomic single-layer Pt in NH3 oxidation 原子单层Pt在NH3氧化中的羟基锚定和电子转移行为
IF 9.4
Chem Catalysis Pub Date : 2025-09-23 DOI: 10.1016/j.checat.2025.101521
Xing Yuan, Wenzhe Si, Xiao Zhu, Bin Zhou, Yue Peng, Junhua Li
{"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}
引用次数: 0
Dual-polarity engineering breaks charge transfer kinetic balances to enhance H2O2-mediated nitrate photosynthesis from air 双极性工程打破电荷转移动力学平衡,增强空气中h2o2介导的硝酸盐光合作用
IF 9.4
Chem Catalysis Pub Date : 2025-09-23 DOI: 10.1016/j.checat.2025.101513
Yunxia Liu, Xiaoxu Deng, Shuo Geng, Shuang-Feng Yin, Peng Chen
{"title":"Dual-polarity engineering breaks charge transfer kinetic balances to enhance H2O2-mediated nitrate photosynthesis from air","authors":"Yunxia Liu, Xiaoxu Deng, Shuo Geng, Shuang-Feng Yin, Peng Chen","doi":"10.1016/j.checat.2025.101513","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101513","url":null,"abstract":"Sustainable H<sub>2</sub>O<sub>2</sub>-mediated photocatalytic nitrate synthesis from air faces carrier imbalance due to slow hole transfer and ultrafast electron migration. We overcome this by integrating sulfur/oxygen dual-polarity units into electron-deficient naphthalene diimide (NDI)-based donor-acceptor (D-A) π-frameworks, achieving spatiotemporal electron-hole decoupling. Experimental and theoretical analyses indicate that this dual-polarity architecture gives rise to tandem endogenous electric fields and robust macroscopic polarization, creating spatially separated “electron platforms” and “hole superchannels,” which reduce recombination and accelerate redox kinetics. Crucially, polarization-induced ordered molecular alignment aligns reactant orientations and lowers N≡N dissociation barriers, enabling concurrent oxygen reduction and nitrogen oxidation. The optimized catalyst achieves a record nitrate yield of 8.89 mg g<sup>−1</sup> h<sup>−1</sup> with an apparent quantum efficiency of 5.50%, outperforming state-of-the-art metal-free systems. Our work introduces innovative design principles and offers a profound perspective for achieving differential bidirectional control over electron and hole carrier transfer rates.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"190 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145116674","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}
引用次数: 0
Shaping the future of green methanol 塑造绿色甲醇的未来
IF 9.4
Chem Catalysis Pub Date : 2025-09-18 DOI: 10.1016/j.checat.2025.101515
Xinyue Cui, Deshan Hou, Qiming Bing, Jingting Hu, Dehui Deng
{"title":"Shaping the future of green methanol","authors":"Xinyue Cui, Deshan Hou, Qiming Bing, Jingting Hu, Dehui Deng","doi":"10.1016/j.checat.2025.101515","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101515","url":null,"abstract":"Methanol, a crucial platform chemical and alternative fuel, has recently gained recognition as a promising hydrogen-storage carrier. The global transition toward carbon-neutral economies, reinforced by increasingly stringent environmental regulations, is driving interest in green methanol synthesis based on renewable hydrogen (produced through water electrolysis powered by renewable energy) and captured CO<sub>2</sub> feedstock. This power-to-liquid technology represents a paradigm shift in chemical manufacturing by effectively converting intermittent renewable electricity into a storable liquid fuel or chemical while enabling a closed-loop carbon cycle. This perspective examines the past, present, and future of methanol synthesis from CO<sub>2</sub> hydrogenation with a particular emphasis on catalyst and process development, the concept of green methanol, CO<sub>2</sub> and H<sub>2</sub> sources, and economic considerations. We conclude by discussing the future prospects of CO<sub>2</sub> hydrogenation to green methanol with the aim of inspiring critical insights and further research in this field.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"38 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145078499","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}
引用次数: 0
From fragile interfaces to armored networks in protonic ceramic electrochemical cells 从脆弱的界面到质子陶瓷电化学电池的装甲网络
IF 9.4
Chem Catalysis Pub Date : 2025-09-18 DOI: 10.1016/j.checat.2025.101514
Yunfei Bu, Zhibin Yang
{"title":"From fragile interfaces to armored networks in protonic ceramic electrochemical cells","authors":"Yunfei Bu, Zhibin Yang","doi":"10.1016/j.checat.2025.101514","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101514","url":null,"abstract":"In the July issue of <em>Nature Energy</em>, Liu and co-workers report a conformally coated scaffold (CCS) oxygen-electrode architecture that enables protonic ceramic electrochemical cells (PCECs) to operate stably for over 5,000 h at −1.5 A cm<sup>−2</sup> under 40% H<sub>2</sub>O at 600°C. The CCS design, based on the water-tolerant, triple-conducting Ruddlesden-Popper oxide Pr<sub>1.8</sub>Ba<sub>0.2</sub>NiO<sub>4+</sub>δ (PBNO), mitigates electrolyte degradation and improves interfacial charge transfer, advancing PCEC durability and performance toward practical application.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"1 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145078495","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}
引用次数: 0
Reactant-induced self-adaptive Pd/Nb2O5 catalyst for alkyne semi-hydrogenation 反应物诱导的自适应Pd/Nb2O5炔半加氢催化剂
IF 9.4
Chem Catalysis Pub Date : 2025-09-18 DOI: 10.1016/j.checat.2025.101522
Jiani Zhang, Risheng Bai
{"title":"Reactant-induced self-adaptive Pd/Nb2O5 catalyst for alkyne semi-hydrogenation","authors":"Jiani Zhang, Risheng Bai","doi":"10.1016/j.checat.2025.101522","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101522","url":null,"abstract":"In the August issue of <em>Cell Reports Physical Science</em>, Yao, Dai, Wang, and co-workers develop a self-adaptive Pd/Nb<sub>2</sub>O<sub>5</sub> catalyst that dynamically reconstructs its interface for aliphatic alkynes but remains stable for aromatic ones. This intelligent modulation induces an attritionary active site, enabling a 40-fold higher reaction rate than the Lindlar catalyst and breaking the activity-selectivity trade-off.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"11 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145078494","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}
引用次数: 0
Access to chiral spiroketals via catalytic enantioselective halogenation of racemic olefinic hemiketals 外消旋烯烃半酮催化对映选择性卤化制备手性螺旋酮
IF 9.4
Chem Catalysis Pub Date : 2025-09-16 DOI: 10.1016/j.checat.2025.101512
Rui Chen, Yuzhuo Liu, Haihui Wang, Ying-Lung Steve Tse, Ying-Yeung Yeung
{"title":"Access to chiral spiroketals via catalytic enantioselective halogenation of racemic olefinic hemiketals","authors":"Rui Chen, Yuzhuo Liu, Haihui Wang, Ying-Lung Steve Tse, Ying-Yeung Yeung","doi":"10.1016/j.checat.2025.101512","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101512","url":null,"abstract":"Chiral spiroketals are privileged structural motifs that widely appear in natural products, pharmaceutical agents, and chiral catalysts. Nevertheless, catalytic asymmetric methods for synthesizing chiral spiroketals remain scarce. Here, we report an asymmetric catalytic halogenation of racemic olefinic hemiketals to synthesize chiral halo-spiroketals. The approach utilizes a cross-assembled bifunctional catalyst system that integrates a chiral phosphoric acid with an achiral quinoline base. Optimization of the reaction was accomplished mainly by modifying the cost-effective achiral quinoline. The reaction mechanism is characterized by a dynamic kinetic resolution of hemiketal and a diastereoselective bromocyclization, underscoring the critical function of the achiral quinoline base throughout both phases of the catalytic process. The chiral halo-spiroketals are important intermediates for the synthesis of chiral spiroketal phosphine ligands, which can be applied in various asymmetric catalytic reactions. The halogen substituents in the spiroketal phosphine ligands enable late-stage modifications that aid in the selection of suitable ligands for particular reactions.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"46 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145068131","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}
引用次数: 0
Breaking the conversion-selectivity trade-off through a plasma reaction-separation coupling process 通过等离子体反应-分离耦合过程打破转换-选择性权衡
IF 9.4
Chem Catalysis Pub Date : 2025-09-15 DOI: 10.1016/j.checat.2025.101498
Lu Wang, Xin Wang, Yutian Li, Zean Xie, Wencui Li, Dong Li, Yangyang Song, Yanhui Yi, Zhen Zhao
{"title":"Breaking the conversion-selectivity trade-off through a plasma reaction-separation coupling process","authors":"Lu Wang, Xin Wang, Yutian Li, Zean Xie, Wencui Li, Dong Li, Yangyang Song, Yanhui Yi, Zhen Zhao","doi":"10.1016/j.checat.2025.101498","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101498","url":null,"abstract":"Using CH<sub>4</sub> under ambient conditions remains a major challenge. Although energetic electrons in non-thermal plasma can activate their C–H chemical bonds at ambient temperature and pressure, the target oxygenates are more reactive than the reactants, inevitably leading to excessive oxidation in the plasma. The limited yield restricts their industrial application. Herein, we have designed a plasma reaction mode to realize a plasma reaction-separation coupling technology capable of protecting intermediate products through facile separation to break the conversion-selectivity trade-off. Coupling the high-space-velocity cyclic process with plasma technology can further increase the yield of liquid fuel and reduce the formation of the overoxidation product CO<sub>2</sub>. This advancement strengthens the viability of plasma for the selective oxidation of methane for industrial applications.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"22 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145059607","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}
引用次数: 0
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