Pub Date : 2026-01-07DOI: 10.1038/s41929-025-01472-w
Li-Wen Wu, Pin-Tian Lyu, Ran Zhang, Keng Chen, Li Zuo, Dongliang Song, Zhen-Zhen Feng, Ya-Ting Nie, Xiaodong Cheng, Teng-Xiang Huang, Bin Kang, Ning Fang
Photogenerated charge carriers play a pivotal role in driving chemical transformations during photocatalysis. However, the structural complexity of photocatalysts presents challenges in establishing nanoscale correlation between carrier dynamics and photocatalytic activity. Here we integrate single-molecule fluorescence imaging with femtosecond interferometric scattering microscopy to resolve the carrier dynamics and specific reaction rate of hydroxyl radical oxidation at the individual structural features (that is, basal plane, edge and wrinkle) in 2D layered indium selenide (InSe). We find a positive linear correlation between the specific reaction rate and the carrier lifetime, but only a weak correlation with the carrier concentration. Moreover, both basal planes and edges exhibit peak lifetimes and specific reaction rates in three-layer InSe. These spatially resolved, correlative single-molecule superlocalization and ultrafast measurements are a powerful tool for investigations of structure–function correlation. Monitoring charge carrier dynamics and photocatalytic reaction rates in individual photocatalyst particles is a challenging task that can help us to understand structure–reactivity relationships. Here single-molecule fluorescence imaging is coupled with femtosecond interferometric scattering microscopy to investigate these properties in 2D InSe flakes.
{"title":"Nanoscale correlation of single-molecule reactivity and charge carrier dynamics in a two-dimensional layered InSe photocatalyst","authors":"Li-Wen Wu, Pin-Tian Lyu, Ran Zhang, Keng Chen, Li Zuo, Dongliang Song, Zhen-Zhen Feng, Ya-Ting Nie, Xiaodong Cheng, Teng-Xiang Huang, Bin Kang, Ning Fang","doi":"10.1038/s41929-025-01472-w","DOIUrl":"10.1038/s41929-025-01472-w","url":null,"abstract":"Photogenerated charge carriers play a pivotal role in driving chemical transformations during photocatalysis. However, the structural complexity of photocatalysts presents challenges in establishing nanoscale correlation between carrier dynamics and photocatalytic activity. Here we integrate single-molecule fluorescence imaging with femtosecond interferometric scattering microscopy to resolve the carrier dynamics and specific reaction rate of hydroxyl radical oxidation at the individual structural features (that is, basal plane, edge and wrinkle) in 2D layered indium selenide (InSe). We find a positive linear correlation between the specific reaction rate and the carrier lifetime, but only a weak correlation with the carrier concentration. Moreover, both basal planes and edges exhibit peak lifetimes and specific reaction rates in three-layer InSe. These spatially resolved, correlative single-molecule superlocalization and ultrafast measurements are a powerful tool for investigations of structure–function correlation. Monitoring charge carrier dynamics and photocatalytic reaction rates in individual photocatalyst particles is a challenging task that can help us to understand structure–reactivity relationships. Here single-molecule fluorescence imaging is coupled with femtosecond interferometric scattering microscopy to investigate these properties in 2D InSe flakes.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 1","pages":"87-94"},"PeriodicalIF":44.6,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145908193","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-06DOI: 10.1038/s41929-025-01463-x
Yang Bai, Kangming Li, Ning Han, Jiheon Kim, Runze Zhang, Suhas Mahesh, Ali Shayesteh Zeraati, Brandon R. Sutherland, Kelvin Chow, Yongxiang Liang, Sjoerd Hoogland, Jianan Erick Huang, David Sinton, Edward H. Sargent, Jason Hattrick-Simpers
Ruthenium oxides (RuOx) are promising alternatives to iridium catalysts for the oxygen-evolution reaction in proton-exchange membrane water electrolysis but lack stability in acid. Alloying with other elements can improve stability and performance but enlarges the search space. Material acceleration platforms combining high-throughput experiments with machine learning can accelerate catalyst discovery, yet predicting and co-optimizing synthesizability, activity and stability remain challenging. A predictive featurization workflow that links a hypothesized catalyst to its actual single- or mixed-phase synthesis and acidic oxygen-evolution reaction properties has not been reported. Here we report a hierarchical workflow, termed mixed acceleration, integrating theoretical and experimental descriptors to predict synthesis, activity and stability. Guided by mixed acceleration through 379 experiments, we identified seven ruthenium-based oxides surpassing the Pareto frontier of activity and stability. The most balanced composition, Ru0.5Zr0.1Zn0.4Ox, achieved an overpotential of 194 mV at 10 mA cm−2 with a ruthenium dissolution rate 12 times lower than that of RuO2. Proton-exchange membrane water electrolysers rely on iridium to catalyse their anodic reaction, and while ruthenium is a less costly alternative due to its similar activity, it is not as stable. Now, a hierarchical machine-learning catalyst discovery workflow, termed mixed acceleration, is put forward to predict catalyst synthesis, activity and stability, and identify promising RuOx-based water oxidation catalysts.
钌氧化物（RuOx）是替代铱催化剂用于质子交换膜电解析氧反应的理想催化剂，但在酸性环境中缺乏稳定性。与其他元素结合可以提高稳定性和性能，但会扩大搜索空间。将高通量实验与机器学习相结合的材料加速平台可以加速催化剂的发现，但预测和共同优化合成能力、活性和稳定性仍然具有挑战性。将假设的催化剂与其实际的单相或混合相合成和酸性析氧反应性质联系起来的预测特征工作流尚未被报道。在这里，我们报告了一个分层工作流程，称为混合加速，整合理论和实验描述符来预测合成，活性和稳定性。在混合加速的指导下，通过379次实验，我们确定了7种超越帕累托活性和稳定性边界的钌基氧化物。最平衡的组合物Ru0.5Zr0.1Zn0.4Ox在10 mA cm−2下的过电位为194 mV，钌的溶解速度比RuO2低12倍。质子交换膜水电解器依靠铱来催化它们的阳极反应，而钌是一种成本较低的替代品，因为它具有类似的活性，但它不那么稳定。现在，提出了一种分层机器学习催化剂发现工作流程，称为混合加速，用于预测催化剂的合成、活性和稳定性，并识别有前途的基于ruox的水氧化催化剂。
{"title":"Stable acidic oxygen-evolving catalyst discovery through mixed accelerations","authors":"Yang Bai, Kangming Li, Ning Han, Jiheon Kim, Runze Zhang, Suhas Mahesh, Ali Shayesteh Zeraati, Brandon R. Sutherland, Kelvin Chow, Yongxiang Liang, Sjoerd Hoogland, Jianan Erick Huang, David Sinton, Edward H. Sargent, Jason Hattrick-Simpers","doi":"10.1038/s41929-025-01463-x","DOIUrl":"10.1038/s41929-025-01463-x","url":null,"abstract":"Ruthenium oxides (RuOx) are promising alternatives to iridium catalysts for the oxygen-evolution reaction in proton-exchange membrane water electrolysis but lack stability in acid. Alloying with other elements can improve stability and performance but enlarges the search space. Material acceleration platforms combining high-throughput experiments with machine learning can accelerate catalyst discovery, yet predicting and co-optimizing synthesizability, activity and stability remain challenging. A predictive featurization workflow that links a hypothesized catalyst to its actual single- or mixed-phase synthesis and acidic oxygen-evolution reaction properties has not been reported. Here we report a hierarchical workflow, termed mixed acceleration, integrating theoretical and experimental descriptors to predict synthesis, activity and stability. Guided by mixed acceleration through 379 experiments, we identified seven ruthenium-based oxides surpassing the Pareto frontier of activity and stability. The most balanced composition, Ru0.5Zr0.1Zn0.4Ox, achieved an overpotential of 194 mV at 10 mA cm−2 with a ruthenium dissolution rate 12 times lower than that of RuO2. Proton-exchange membrane water electrolysers rely on iridium to catalyse their anodic reaction, and while ruthenium is a less costly alternative due to its similar activity, it is not as stable. Now, a hierarchical machine-learning catalyst discovery workflow, termed mixed acceleration, is put forward to predict catalyst synthesis, activity and stability, and identify promising RuOx-based water oxidation catalysts.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 1","pages":"28-36"},"PeriodicalIF":44.6,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145903494","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-06DOI: 10.1038/s41929-025-01462-y
Yaohang Cheng, Chengyihan Gu, Jie Han, Yulan Chen, Yuxi Tian, Chengjian Zhu, Jin Xie
Radical ligand transfer (RLT), a process in which alkyl radicals capture ligands from high-valent metal species, has emerged as a powerful synthetic approach in organic chemistry. While RLT processes mediated by 3d transition metals have been developed, the application of 5d transition metals remains underexplored due to the limited flexibility in their oxidation states. Here we present a catalytic approach leveraging sequential photoinduced electron transfer in dinuclear gold complexes to achieve an efficient RLT process. This strategy facilitates formal additions of gem-dichloroalkanes and Freon-22 bearing unactivated C(sp3)–Cl bonds to different kinds of alkenes, with high reactivity, excellent atom economy and broad scope. Combined mechanistic and theoretical investigations reveal a latent AuIIAuII pathway. The success originates from sequential excitation of dinuclear gold complexes for the formation of a covalent Au–Au bond, which can markedly weaken the Au–Cl bond and facilitate ligand transfer. Radical ligand transfer is a common reactive pathway in 3d transition metals. Here the authors describe it for 5d transition metals in dinuclear gold complexes, for the formal addition of unactivated C(sp3)–Cl bond in gem-dichloroalkanes and Freon-22 to different kinds of alkenes.
{"title":"Radical ligand transfer catalysis of photoexcited dinuclear gold complexes","authors":"Yaohang Cheng, Chengyihan Gu, Jie Han, Yulan Chen, Yuxi Tian, Chengjian Zhu, Jin Xie","doi":"10.1038/s41929-025-01462-y","DOIUrl":"10.1038/s41929-025-01462-y","url":null,"abstract":"Radical ligand transfer (RLT), a process in which alkyl radicals capture ligands from high-valent metal species, has emerged as a powerful synthetic approach in organic chemistry. While RLT processes mediated by 3d transition metals have been developed, the application of 5d transition metals remains underexplored due to the limited flexibility in their oxidation states. Here we present a catalytic approach leveraging sequential photoinduced electron transfer in dinuclear gold complexes to achieve an efficient RLT process. This strategy facilitates formal additions of gem-dichloroalkanes and Freon-22 bearing unactivated C(sp3)–Cl bonds to different kinds of alkenes, with high reactivity, excellent atom economy and broad scope. Combined mechanistic and theoretical investigations reveal a latent AuIIAuII pathway. The success originates from sequential excitation of dinuclear gold complexes for the formation of a covalent Au–Au bond, which can markedly weaken the Au–Cl bond and facilitate ligand transfer. Radical ligand transfer is a common reactive pathway in 3d transition metals. Here the authors describe it for 5d transition metals in dinuclear gold complexes, for the formal addition of unactivated C(sp3)–Cl bond in gem-dichloroalkanes and Freon-22 to different kinds of alkenes.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 1","pages":"18-27"},"PeriodicalIF":44.6,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145903493","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 10.1038/s41929-025-01460-0
Volker Derdau
Deuterated compounds find applications in a variety of fields including catalysis optimization, mass spectrometry standards, pharmaceutical development and organic light emitting diodes. A recent study indicates that the choice of deuterium source significantly affects both the outcomes and mechanistic pathways in catalytic cycles.
{"title":"The deuterium source matters","authors":"Volker Derdau","doi":"10.1038/s41929-025-01460-0","DOIUrl":"10.1038/s41929-025-01460-0","url":null,"abstract":"Deuterated compounds find applications in a variety of fields including catalysis optimization, mass spectrometry standards, pharmaceutical development and organic light emitting diodes. A recent study indicates that the choice of deuterium source significantly affects both the outcomes and mechanistic pathways in catalytic cycles.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 12","pages":"1264-1265"},"PeriodicalIF":44.6,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145808780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 10.1038/s41929-025-01461-z
Nitish Govindarajan, An T. Chu, Christopher Hahn, Yogesh Surendranath
Electrocatalysts enable the efficient interconversion of electrical and chemical energy for the sustainable production of fuels and chemicals. Here we highlight the importance of developing electrochemical adsorption isotherms to demystify complex reaction mechanisms and rationalize catalytic activity.
{"title":"The overlooked role of adsorption isotherms in electrocatalysis","authors":"Nitish Govindarajan, An T. Chu, Christopher Hahn, Yogesh Surendranath","doi":"10.1038/s41929-025-01461-z","DOIUrl":"10.1038/s41929-025-01461-z","url":null,"abstract":"Electrocatalysts enable the efficient interconversion of electrical and chemical energy for the sustainable production of fuels and chemicals. Here we highlight the importance of developing electrochemical adsorption isotherms to demystify complex reaction mechanisms and rationalize catalytic activity.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 12","pages":"1254-1259"},"PeriodicalIF":44.6,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145808781","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 10.1038/s41929-025-01458-8
Cong Xiao, Wen-Jing Xiao
Energy transfer photocatalysis typically requires expensive metal complexes or specific synthetic photosensitizers with particular triplet energies. Nitroarenes now emerge as powerful, sustainable alternatives, with their catalytic efficiency governed by excited-state geometry rather than only by energy matching, enabling efficient alkene isomerizations and cycloadditions.
{"title":"Nitroarenes as energy transfer catalysts","authors":"Cong Xiao, Wen-Jing Xiao","doi":"10.1038/s41929-025-01458-8","DOIUrl":"10.1038/s41929-025-01458-8","url":null,"abstract":"Energy transfer photocatalysis typically requires expensive metal complexes or specific synthetic photosensitizers with particular triplet energies. Nitroarenes now emerge as powerful, sustainable alternatives, with their catalytic efficiency governed by excited-state geometry rather than only by energy matching, enabling efficient alkene isomerizations and cycloadditions.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 12","pages":"1260-1261"},"PeriodicalIF":44.6,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145808782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 10.1038/s41929-025-01457-9
Jianbin Li, Ding Zhang, Zhennan Hu, Zehao Yuan
Photocatalysis has become a cornerstone in modern organic synthesis due to its ability to generate and manage reactive radical intermediates, thus facilitating diverse chemical processes under mild conditions. A critical yet often overlooked aspect of photocatalysis is the dynamic transformation of photocatalysts into their active forms during reactions, which fundamentally governs their reactivity, selectivity and reaction outcome. Here we term this class of catalysts ‘transformer photocatalysts’, which undergo various activation pathways such as reductive activation, acid coordination, radical substitution and deconstructive processes. By categorizing selected examples based on these activation mechanisms, we aim to highlight the typical activation modes of some common photocatalysts and elucidate the underlying principles that guide the formation and behaviour of these active species. We hope that these mechanistic insights will provide a foundation for broadening the horizon of photocatalysis and developing photocatalysts tailored to organic transformations, thus inspiring further research in photochemistry and beyond. Photocatalysis enables many appealing synthetic reactions to proceed under mild conditions. This Review focuses on structural and electronic changes of photocatalysts, potentially resulting in frequently neglected active species that facilitate catalysis.
{"title":"Illuminating the transformation of photocatalysts in light-driven organic synthesis","authors":"Jianbin Li, Ding Zhang, Zhennan Hu, Zehao Yuan","doi":"10.1038/s41929-025-01457-9","DOIUrl":"10.1038/s41929-025-01457-9","url":null,"abstract":"Photocatalysis has become a cornerstone in modern organic synthesis due to its ability to generate and manage reactive radical intermediates, thus facilitating diverse chemical processes under mild conditions. A critical yet often overlooked aspect of photocatalysis is the dynamic transformation of photocatalysts into their active forms during reactions, which fundamentally governs their reactivity, selectivity and reaction outcome. Here we term this class of catalysts ‘transformer photocatalysts’, which undergo various activation pathways such as reductive activation, acid coordination, radical substitution and deconstructive processes. By categorizing selected examples based on these activation mechanisms, we aim to highlight the typical activation modes of some common photocatalysts and elucidate the underlying principles that guide the formation and behaviour of these active species. We hope that these mechanistic insights will provide a foundation for broadening the horizon of photocatalysis and developing photocatalysts tailored to organic transformations, thus inspiring further research in photochemistry and beyond. Photocatalysis enables many appealing synthetic reactions to proceed under mild conditions. This Review focuses on structural and electronic changes of photocatalysts, potentially resulting in frequently neglected active species that facilitate catalysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 12","pages":"1268-1280"},"PeriodicalIF":44.6,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145808783","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 10.1038/s41929-025-01455-x
Boon Siang Yeo
Electrocatalytic CO2 reduction on Cu is typically studied at room temperature and pressure, producing mostly C1 and C2 products (short carbon chains). High-temperature experiments above 125 °C now reveal a carbon-chain growth mechanism akin to the thermally driven Fischer–Tropsch reaction, resulting in the production of C1–C5 hydrocarbons.
{"title":"Growing the carbon chain","authors":"Boon Siang Yeo","doi":"10.1038/s41929-025-01455-x","DOIUrl":"10.1038/s41929-025-01455-x","url":null,"abstract":"Electrocatalytic CO2 reduction on Cu is typically studied at room temperature and pressure, producing mostly C1 and C2 products (short carbon chains). High-temperature experiments above 125 °C now reveal a carbon-chain growth mechanism akin to the thermally driven Fischer–Tropsch reaction, resulting in the production of C1–C5 hydrocarbons.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 12","pages":"1266-1267"},"PeriodicalIF":44.6,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145808788","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-12-22DOI: 10.1038/s41929-025-01468-6
Marcal Capdevila-Cortada
{"title":"Shifting both ways on ceria","authors":"Marcal Capdevila-Cortada","doi":"10.1038/s41929-025-01468-6","DOIUrl":"10.1038/s41929-025-01468-6","url":null,"abstract":"","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"8 12","pages":"1252-1252"},"PeriodicalIF":44.6,"publicationDate":"2025-12-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145808785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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