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Performance-enhancing asymmetric catalysis unlocks tuning without rebuilding 提高性能的不对称催化无需重建即可解锁调优
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-19 DOI: 10.1016/j.checat.2025.101577
Zihang Deng, Jeffrey N. Johnston
Zihang Deng received his PhD degree from Vanderbilt University, where his research focused on developing asymmetric organocatalyst generality and employing high-throughput screening in organocatalysis. He is currently a postdoctoral scholar at Harvard University (with Richard Liu), where he develops innovative coupling reagents for bioconjugation.Jeffrey N. Johnston is a Stevenson Professor of Chemistry at Vanderbilt University, where he leads a research program that develops new reactions and reagents for the synthesis of complex natural products and therapeutics. The integrative design of sustainable catalysts with strategic fragment-assembling schemes and the acceleration of the discovery phase in enantioselective catalysis are high priorities.
邓子航博士毕业于美国范德比尔特大学,主要研究方向为不对称有机催化剂的开发及在有机催化中的高通量筛选。他目前是哈佛大学博士后学者(与Richard Liu合作),在那里他开发了用于生物偶联的创新偶联试剂。Jeffrey N. Johnston是Vanderbilt University的史蒂文森化学教授,在那里他领导一个研究项目,开发用于合成复杂天然产物和治疗的新反应和试剂。可持续催化剂与战略性片段组装方案的整合设计和加速对映选择性催化的发现阶段是当务之急。
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引用次数: 0
Iridium management strategies for scalable proton exchange membrane water electrolysis 可扩展质子交换膜电解的铱管理策略
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-18 DOI: 10.1016/j.checat.2025.101570
Kexin Zhang, Xinyue Ni, Xiao Liang, Xiaoxin Zou
Proton exchange membrane water electrolysis (PEMWE) is increasingly recognized as a key technology for green hydrogen production in support of global decarbonization efforts. However, its large-scale deployment remains constrained by the reliance on scarce iridium (Ir) as the anode catalyst. While recent advances in anode catalyst design have improved Ir utilization, long-term scalability requires a more comprehensive Ir management approach. This perspective presents an integrated strategy for scalable PEMWE combining improved utilization and closed-loop recycling. We summarize current progress in anode catalyst innovation, catalyst layer architecture, and non-catalyst-component optimization, with a particular emphasis on the urgency and technical feasibility of Ir recovery to align with future deployment scenarios. To realize the full potential of green hydrogen, we call for the adoption of this integrated Ir management framework across research, industry, and policy domains.
质子交换膜水电解(PEMWE)越来越被认为是支持全球脱碳努力的绿色制氢的关键技术。然而,它的大规模部署仍然受到依赖稀缺的铱(Ir)作为阳极催化剂的限制。虽然阳极催化剂设计的最新进展提高了Ir利用率,但长期可扩展性需要更全面的Ir管理方法。这一观点提出了一种可扩展的PEMWE综合策略,结合了提高利用率和闭环回收。我们总结了阳极催化剂创新、催化剂层结构和非催化剂组分优化方面的最新进展,特别强调了Ir回收的紧迫性和技术可行性,以配合未来的部署方案。为了充分发挥绿色氢的潜力,我们呼吁在研究、工业和政策领域采用这种综合的氢管理框架。
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引用次数: 0
Light-controlled active-site engineering in photo-thermal catalysis 光热催化中的光控活性位点工程
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-18 DOI: 10.1016/j.checat.2025.101569
Diego Mateo, Enrique V. Ramos-Fernandez, Jorge Gascon
Photo-adaptive catalysis enables dynamic modulation of catalytic activity and selectivity using light as an external stimulus. When coupled with photo-thermal processes, it allows precise control over thermal and non-thermal light contributions to catalytic performance. This viewpoint critically examines recent advances in heterogeneous photo-switchable systems, emphasizing light-induced structural and electronic transformations such as reversible vacancy generation and redox dynamics in plasmonic metals. Particular attention is given to the synergy between photonic and thermal effects that govern the transient nature of active sites. We also discuss progress in operando characterization techniques capable of capturing fast structural and electronic changes, together with challenges related to reactor engineering, material stability, and scalability. Overall, integrating dynamic light control with heterogeneous catalysis provides a path toward programmable catalytic systems for demanding transformations, such as CO2 hydrogenation and ammonia synthesis.
光自适应催化可以利用光作为外部刺激对催化活性和选择性进行动态调节。当与光热过程相结合时,它可以精确控制对催化性能的热和非热光贡献。这一观点批判性地考察了异质光开关系统的最新进展,强调了光诱导的结构和电子转换,如等离子体金属中的可逆空位生成和氧化还原动力学。特别注意的是光子和热效应之间的协同作用,控制活性位点的瞬态性质。我们还讨论了能够捕捉快速结构和电子变化的operando表征技术的进展,以及与反应堆工程、材料稳定性和可扩展性相关的挑战。总的来说,将动态光控制与多相催化相结合,为要求苛刻的转化(如CO2加氢和氨合成)提供了一条通往可编程催化系统的途径。
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引用次数: 0
Lead-free Cs2AgBiBr6 double-perovskite nanoplatelets as photocatalysts for solid-phase oxidation of 1,2-benzenedimethanol 无铅Cs2AgBiBr6双钙钛矿纳米片作为1,2-苯二甲醇固相氧化的光催化剂
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-11 DOI: 10.1016/j.checat.2025.101566
Rongzhen Wu, Tong Cai, Zhenyang Liu, Xinfeng Chen, Yasutaka Nagaoka, Paul G. Williard, Ou Chen
We report the first application of lead-free Cs2AgBiBr6 double-perovskite nanoplatelets as efficient photocatalysts for solid-phase photooxidation reactions. These 2D nanomaterials exhibit excellent performance in the solvent-free ring-closing oxidation of 1,2-benzenedimethanol, achieving a remarkable yield of 98.2%. The high catalytic activity is attributed to the large, exposed surface area and favorable catalyst-substrate interactions. Mechanistic investigations, including radical trapping experiments, reveal a free-radical-driven oxidation pathway. This study extends the applications of halide perovskite nanomaterials in polar organic substrate catalysis by eliminating the need for a polar solvent environment, demonstrating the promising potential of lead-free halide perovskites in solid-phase photocatalysis while providing fundamental insights into their applications for sustainable chemical transformations.
我们报道了无铅Cs2AgBiBr6双钙钛矿纳米片作为固相光氧化反应的高效光催化剂的首次应用。这些二维纳米材料在1,2-苯二甲醇的无溶剂闭环氧化中表现出优异的性能,收率达到了98.2%。高催化活性归因于大的暴露表面积和良好的催化剂-底物相互作用。机理研究,包括自由基捕获实验,揭示了自由基驱动的氧化途径。本研究通过消除极性溶剂环境的需要,扩展了卤化物钙钛矿纳米材料在极性有机底物催化中的应用,展示了无铅卤化物钙钛矿在固相光催化中的广阔潜力,同时为其在可持续化学转化中的应用提供了基本见解。
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引用次数: 0
In situ Raman study of oxygen reduction reactions on model and nanocatalysts 模型和纳米催化剂上氧还原反应的原位拉曼研究
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-11-11 DOI: 10.1016/j.checat.2025.101565
Xiao-Yan Huang, Run-Ze Zhang, Lie Zou, Yi Zhang, Jin-Feng Li, Ze-Yu Zhang, Hua Zhang, Qing-Chi Xu, Jian-Feng Li
The oxygen reduction reaction (ORR) is the cathodic process in fuel cells. Due to its slow kinetics, developing more active catalysts while minimizing fuel cell production costs is crucial. Monitoring intermediate species during the reaction would promote fundamental understanding of the ORR mechanism and rational design of better catalysts. This review goes over the application of in situ surface-enhanced Raman spectroscopy (SERS) to reveal the ORR mechanisms across various catalysts, such as single-crystal electrodes, nanocatalysts, and single-atom catalysts (SACs). It covers techniques like the “borrowing” SERS strategy, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), and tip-enhanced Raman spectroscopy (TERS) used in ORR studies. These methods enable in situ observation of reaction intermediates and active sites. The insights gained contribute to understanding the fundamental ORR processes and aid in designing more effective catalysts. Additionally, this work can serve as a reference for investigating other electrocatalytic reaction mechanisms.
氧还原反应(ORR)是燃料电池中的阴极反应。由于其缓慢的动力学,开发更多的活性催化剂,同时最小化燃料电池的生产成本是至关重要的。监测反应过程中的中间物质有助于对ORR机理的基本认识和合理设计更好的催化剂。本文综述了原位表面增强拉曼光谱(SERS)在不同催化剂上的应用,如单晶电极、纳米催化剂和单原子催化剂(SACs)。它涵盖了“借用”SERS策略、壳隔离纳米粒子增强拉曼光谱(SHINERS)和ORR研究中使用的尖端增强拉曼光谱(TERS)等技术。这些方法能够对反应中间体和活性位点进行现场观察。所获得的见解有助于理解基本的ORR过程,并有助于设计更有效的催化剂。此外,本研究也可为其他电催化反应机理的研究提供参考。
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引用次数: 0
Mixed-anion materials as an emerging material platform for photocatalysis 混合阴离子材料作为光催化的新兴材料平台
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-10-16 DOI: 10.1016/j.checat.2025.101520
Jill K. Wenderott
Jill K. Wenderott is the Anne Stevens Assistant Professor of Materials Science and Engineering at Drexel University, where her research group focuses on informed synthesis of functional inorganic materials for use in energy and environmental applications. She completed her BS in physics at the University of Kansas before receiving her PhD in materials science and engineering from the University of Michigan. After her PhD, she was a postdoc in the Department of Materials Science and Engineering at Northwestern University and subsequently a postdoctoral appointee at Argonne National Laboratory in the Materials Science Division.
吉尔·温德洛特是德雷塞尔大学材料科学与工程的安妮·史蒂文斯助理教授,她的研究小组专注于在能源和环境应用中使用的功能性无机材料的合成。她在堪萨斯大学获得物理学学士学位,然后在密歇根大学获得材料科学与工程博士学位。博士毕业后,她在美国西北大学材料科学与工程系担任博士后,随后在美国阿贡国家实验室材料科学部担任博士后。
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引用次数: 0
Techno-economic assessment of non-aqueous CO2 reduction 非水CO2减排技术经济评价
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-10-16 DOI: 10.1016/j.checat.2025.101548
Shashwati C. da Cunha, Joaquin Resasco
Most research on low-temperature CO2 electrolysis has focused on aqueous electrolytes, primarily because non-aqueous systems require high cell voltages. However, CO2 reduction (CO2R) in aqueous electrolytes competes with hydrogen evolution and requires many electron transfers to produce C2+ molecules, challenges that can be mitigated in non-aqueous electrolytes. In this forward-looking techno-economic assessment, we model the costs of non-aqueous CO2R. We show that CO2R to oxalic acid—a two-electron C2 product formed in aprotic electrolytes—is surprisingly affordable, although non-aqueous CO production is expensive. Using parameters from the largest collection of literature data on CO2R in aprotic non-aqueous electrolytes, we find that oxalic acid would cost $2.87/kgoxalic acid in a small-scale process. A commercial-scale plant would lower the product cost to $1.56/kgoxalic acid, approaching current market prices. Capital costs are dominated by product separation and operating costs mostly by stack replacement and electricity to drive the high required cell voltage. We present a roadmap toward cost-competitive non-aqueous CO2R to oxalic acid, a pathway to scale-up that has been overlooked compared to aqueous CO2 electrolysis.
大多数关于低温CO2电解的研究都集中在水电解质上,主要是因为非水系统需要高电池电压。然而,水电解质中的CO2还原(CO2R)与析氢相竞争,并且需要许多电子转移来产生C2+分子,这在非水电解质中可以减轻挑战。在这个前瞻性的技术经济评估中,我们模拟了非水CO2R的成本。我们表明,CO2R生成草酸是一种在非质子电解质中形成的双电子C2产物,尽管非水CO生产成本昂贵,但其价格却令人惊讶地便宜。利用非质子非水电解质中CO2R的最大文献数据集的参数,我们发现在小规模工艺中,草酸的成本为2.87美元/ kgo草酸。一个商业规模的工厂将把产品成本降低到1.56美元/克草酸,接近目前的市场价格。资本成本主要是产品分离和运营成本主要是堆叠更换和电力驱动所需的高电池电压。我们提出了一个具有成本竞争力的非水CO2R制草酸的路线图,与水CO2电解相比,这是一个被忽视的扩大规模的途径。
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引用次数: 0
Mediated electrosynthesis for greener ethylene glycol production 绿色乙二醇生产的介导电合成
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-10-16 DOI: 10.1016/j.checat.2025.101549
Ying Yang, Yuyan Wan, Ning Yan
Recently, Sargent’s group reported an efficient route of electrochemical ethylene-to-ethylene glycol conversion via redox mediators with high rate and selectivity. This anodic reaction can be paired with the cathodic CO2 reduction or CO2 capture. In addition to minimizing overall energy consumption, the ingeniously selected cathodic process can optimize the microenvironment at the anode toward higher selectivity and lower electrolysis voltage.
最近,Sargent的团队报道了一种通过氧化还原介质进行电化学乙烯到乙二醇转化的高效途径,具有高速率和选择性。这种阳极反应可以与阴极CO2还原或CO2捕获相结合。除了最大限度地降低总体能耗外,巧妙选择的阴极工艺还可以优化阳极的微环境,使其具有更高的选择性和更低的电解电压。
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引用次数: 0
Pressure-pulsed flow triples mass transport in aqueous CO2 electrolysis 压力脉冲流使含水CO2电解中的质量输运增加了三倍
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-10-16 DOI: 10.1016/j.checat.2025.101547
Jorrit Bleeker, Lisanne C. Bakker, Sue S.J. van Deursen, Timo J.J.M. van Overveld, Katie M.R. Lawrence, Isabell Bagemihl, Giacomo Lastrucci, Duco Bosma, Christiaan V. Schinkel, Evert C. Wagner, J. Ruud van Ommen, David A. Vermaas
Electrochemical CO2 reduction (CO2R) is a promising technology for carbon recycling and energy storage. While gas-fed CO2R is currently the best practice because it facilitates fast mass transport, CO2R in water offers potential advantages such as avoiding salt formation, facile water control, and easier integration with CO2 capture. In this work, we enhance mass transport in an aqueous CO2 electrolyzer using fast pressure pulses (50 Hz, 1.2 bar) with a vibratory pump typically found in coffee machines. We demonstrate a limiting current density of 87 mA cm−2 toward CO2R products—nearly three times higher than without pulses. The current density can be further increased by leveraging the peak-to-peak pressure amplitude or pump frequency, as shown through particle image velocimetry (PIV) and an order-of-magnitude scaling analysis. Although challenges remain, such as pump energy consumption, contamination, heating, and pressure-wave damping, the pressure-pulsed concept is a promising direction for aqueous CO2R.
电化学CO2还原(CO2R)是一种很有前途的碳回收和储能技术。虽然气载CO2R是目前的最佳实践,因为它有助于快速的物质运输,但水中的CO2R具有潜在的优势,如避免盐的形成,易于控制水,更容易与二氧化碳捕获相结合。在这项工作中,我们使用快速压力脉冲(50 Hz, 1.2 bar)和通常在咖啡机中发现的振动泵来增强含水CO2电解槽中的质量输运。我们证明了CO2R产品的极限电流密度为87 mA cm - 2,几乎是没有脉冲的三倍。如粒子图像测速(PIV)和数量级缩放分析所示,可以通过利用峰值压力幅值或泵频进一步提高电流密度。尽管仍存在一些挑战,如泵能耗、污染、加热和压力波阻尼,但压力脉冲的概念是含水CO2R的一个有前途的方向。
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引用次数: 0
Engineering catalytic sites for CO2-to-ethylene photoconversion 二氧化碳到乙烯光转化的工程催化位点
IF 9.4 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-10-16 DOI: 10.1016/j.checat.2025.101539
Devthade Vidyasagar, Wonyong Choi
The selective photoconversion of CO2 to ethylene has been hindered by kinetic and thermodynamic limitations. Two recent studies, published in Nature Catalysis and Nature Communications, reveal how precise control over the geometry and electronic structure of catalytic sites can overcome these bottlenecks to enable record-setting yields for CO2-to-ethylene conversion under mild conditions.
CO2选择性光转化为乙烯受到动力学和热力学限制。最近发表在《自然催化》和《自然通讯》上的两项研究揭示了如何精确控制催化位点的几何形状和电子结构,从而克服这些瓶颈,在温和条件下实现创纪录的二氧化碳-乙烯转化产量。
{"title":"Engineering catalytic sites for CO2-to-ethylene photoconversion","authors":"Devthade Vidyasagar, Wonyong Choi","doi":"10.1016/j.checat.2025.101539","DOIUrl":"https://doi.org/10.1016/j.checat.2025.101539","url":null,"abstract":"The selective photoconversion of CO<sub>2</sub> to ethylene has been hindered by kinetic and thermodynamic limitations. Two recent studies, published in <em>Nature Catalysis</em> and <em>Nature Communications</em>, reveal how precise control over the geometry and electronic structure of catalytic sites can overcome these bottlenecks to enable record-setting yields for CO<sub>2</sub>-to-ethylene conversion under mild conditions.","PeriodicalId":53121,"journal":{"name":"Chem Catalysis","volume":"102 1","pages":""},"PeriodicalIF":9.4,"publicationDate":"2025-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145295433","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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Chem Catalysis
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