Nature Catalysis最新文献

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Porous Ru-loaded covalent organic framework nanofluids for fast and scalable continuous-flow photocatalytic oxidations 用于快速和可扩展的连续流光催化氧化的多孔钌负载共价有机框架纳米流体
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-17 DOI: 10.1038/s41929-026-01555-2
Chao Jiang, Yuhan Wang, Guan Sheng, Yan Liu, Xing Han, Zhongkui Li, Cheng Cheng, Xiangxiang Zhao, Yujie Zhou, Qun Zhang, Minjing Shang, Yihan Zhu, Yuanhai Su, Yong Cui
{"title":"Porous Ru-loaded covalent organic framework nanofluids for fast and scalable continuous-flow photocatalytic oxidations","authors":"Chao Jiang, Yuhan Wang, Guan Sheng, Yan Liu, Xing Han, Zhongkui Li, Cheng Cheng, Xiangxiang Zhao, Yujie Zhou, Qun Zhang, Minjing Shang, Yihan Zhu, Yuanhai Su, Yong Cui","doi":"10.1038/s41929-026-01555-2","DOIUrl":"10.1038/s41929-026-01555-2","url":null,"abstract":"Continuous-flow photocatalysis with heterogeneous catalysts offers a sustainable route for chemical synthesis, but it is limited by catalyst deactivation and inefficient light utilization arising from swelling and pore clogging. Here we develop a high-performance continuous-flow system based on covalent organic framework (COF) nanofluids as porous catalytic dispersions. Two ionic COFs incorporating imine-linked Ru(II)–triphenanthroline photocatalysts are synthesized, featuring triple-helix porous architectures resolved by cryogenic low-dose electron microscopy. Processed into nanofluids with an average particle size below 100 nm, the COFs remain colloidally stable for over seven days without surfactants, enabling efficient mass transfer, light penetration and heat dissipation in flow microreactors. These attributes result in markedly enhanced photocatalytic performance across a range of achiral and chiral oxidation reactions. Notably, artemisinin is produced in 64% yield within 7 min via photooxidation of dihydroartemisinic acid. Integration of a dual-capillary microreactor further doubles productivity, highlighting the scalability and industrial potential of porous nanofluid photocatalysis. Heterogeneous and homogeneous photocatalysts offer different strengths and weaknesses. Here, continuous-flow photocatalytic oxidation reactions are performed using covalent organic framework nanofluids that heterogenize molecular units to combine the advantages of catalyst efficiency, light utilization and easy separation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"666-675"},"PeriodicalIF":48.3,"publicationDate":"2026-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148291279","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}
引用次数: 0
Transient dynamics of flavonoid metabolons tune chalcone synthase specificity 黄酮类代谢的瞬时动态调节查尔酮合成酶的特异性
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-15 DOI: 10.1038/s41929-026-01551-6
Riki Imaizumi, Toshiyuki Waki, Yoshikazu Hattori, Kohei Takeshita, Miru Sumita, Kazutomo Kawaguchi, Hiroyuki Kumeta, Kenichi Umeda, Kyohei Sato, Taro Yanai, Hiroaki Matsuura, Takeshi Yokoyama, Risa Omura, Kayo Nakatani, Naoki Sakai, Yukimura Kawagiwa, Yamato Doi, Aoi Yasuda, Takuya Nakano, Kaichi Uno, Kunihiro Yoshida, Misato Tsunashima, Tomohide Saio, Yoshikazu Tanaka, Seiji Takahashi, Noriyuki Kodera, Kunishige Kataoka, Masaki Yamamoto, Satoshi Yamashita, Toru Nakayama
{"title":"Transient dynamics of flavonoid metabolons tune chalcone synthase specificity","authors":"Riki Imaizumi, Toshiyuki Waki, Yoshikazu Hattori, Kohei Takeshita, Miru Sumita, Kazutomo Kawaguchi, Hiroyuki Kumeta, Kenichi Umeda, Kyohei Sato, Taro Yanai, Hiroaki Matsuura, Takeshi Yokoyama, Risa Omura, Kayo Nakatani, Naoki Sakai, Yukimura Kawagiwa, Yamato Doi, Aoi Yasuda, Takuya Nakano, Kaichi Uno, Kunihiro Yoshida, Misato Tsunashima, Tomohide Saio, Yoshikazu Tanaka, Seiji Takahashi, Noriyuki Kodera, Kunishige Kataoka, Masaki Yamamoto, Satoshi Yamashita, Toru Nakayama","doi":"10.1038/s41929-026-01551-6","DOIUrl":"10.1038/s41929-026-01551-6","url":null,"abstract":"Cells achieve metabolic precision by assembling enzymes into dynamic complexes, but the regulatory mechanism of these metabolons is unclear. Here we characterize the chalcone synthase (CHS)–chalcone isomerase-like protein (CHIL) complex, a key component of flavonoid metabolons. While crystallography provides a static view, our analyses reveal that CHS undergoes rapid, reversible binding cycles with CHIL that regulate catalysis in real time. CHIL removes coenzyme A, an inhibitor of Claisen cyclization, transiently reshapes the CHS active site and guides the tetraketide intermediate towards productive cyclization, thereby suppressing derailment by-products. These findings demonstrate a previously unproven and generalizable regulatory effect in metabolons: guided active-site tuning via transient enzyme association. This concept enhances our understanding of metabolon function and opens avenues for synthetic biology and metabolic engineering. Enzyme assemblies can enhance metabolic efficiency, yet the ways in which transient interactions fine tune catalytic outcomes remain poorly understood. This study demonstrates that a flexible partner protein transiently remodels an enzyme’s active site to favour productive chemistry in a flavonoid metabolon.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"630-644"},"PeriodicalIF":48.3,"publicationDate":"2026-06-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01551-6.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336884","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ammonia splitting with electrode alternating for durable hydrogen production 氨分裂与电极交替,持久制氢
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-11 DOI: 10.1038/s41929-026-01554-3
Tianze Wu, Chencheng Dai, Yuwei Zhang, Yuan Liu, Qian Wu, Kamal Elouarzaki, Fanxu Meng, Xinlong Lin, Mudi Wu, Adrian C. Fisher, Zhichuan J. Xu
{"title":"Ammonia splitting with electrode alternating for durable hydrogen production","authors":"Tianze Wu, Chencheng Dai, Yuwei Zhang, Yuan Liu, Qian Wu, Kamal Elouarzaki, Fanxu Meng, Xinlong Lin, Mudi Wu, Adrian C. Fisher, Zhichuan J. Xu","doi":"10.1038/s41929-026-01554-3","DOIUrl":"10.1038/s41929-026-01554-3","url":null,"abstract":"Ammonia is a promising hydrogen carrier. However, its practical deployment hinges on cost-effective splitting approaches to release hydrogen. Ammonia electrolysis, combining the ammonia oxidation reaction (AOR) and the hydrogen evolution reaction, is a promising decentralized solution that operates under mild conditions. Nevertheless, the susceptibility of nearly all AOR catalysts to severe poisoning compromises activity and stability. Here we show an electrode-alternating approach to regenerate poisoned catalysts in AOR while maintaining high hydrogen productivity. A Pt/C catalyst is chosen for demonstration because it synergizes high intrinsic activity, high regeneration capability and excellent corrosion resistance in electrolytes. Key parameters in electrode alternating, including step time and voltage, are optimized to minimize the hydrogen loss while maximizing productivity. A prototype with electrode alternating (±0.8 V) demonstrates ammonia splitting at a sustained current density of ~2 A cm−2 over 1,000 h, corresponding to a cost of ammonia decomposition to produce H2 at $$sim {rm{US}}{rm{$}}1,{{rm{kg}}}_{{{rm{H}}}_{2}}^{-1}$$ . Electrocatalysts for ammonia oxidation tend to be poisoned by nitrogen-based intermediates. Here the authors use an electrode-alternating strategy that uses pulsed potential reversal to continuously regenerate the deactivated surface, enabling Pt-based ammonia electrolysis for over 1,000 h.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"655-665"},"PeriodicalIF":48.3,"publicationDate":"2026-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148290902","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}
引用次数: 0
Overcoming conformational strain in directed C3-C(sp3)–H activation for saturated azacycles 饱和氮杂环定向C3-C(sp3) -H活化中克服构象应变
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-09 DOI: 10.1038/s41929-026-01549-0
{"title":"Overcoming conformational strain in directed C3-C(sp3)–H activation for saturated azacycles","authors":"","doi":"10.1038/s41929-026-01549-0","DOIUrl":"10.1038/s41929-026-01549-0","url":null,"abstract":"Functionalization of saturated azacycles through Pd-catalysed C3-C(sp3)–H activation leveraging the endocyclic nitrogen as a directing group has been hindered by the intrinsic geometric strain of the palladacycle intermediate. Now, an amine N-oxide strategy overcomes this issue by forming a favourable five-membered palladacycle transition state, enabling selective C3 arylation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"582-583"},"PeriodicalIF":48.3,"publicationDate":"2026-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336876","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}
引用次数: 0
Neutral photogenerated N-centred radicals as a general, catalytic direct hydrogen atom transfer platform for aliphatic C–H functionalization 中性光生成的n中心自由基作为脂肪族碳氢功能化的一般催化直接氢原子转移平台
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-09 DOI: 10.1038/s41929-026-01539-2
Boya Feng  (, ), Mattia Lepori, Michał Domański, Soňa Boháčová, Daniel Bím, Lucie Ludvíková, Tomáš Slanina, Prakash C. Tiwari, Guodong Zhang  (, ), Luigi Dolcini, Timothy Noël, Joshua P. Barham
{"title":"Neutral photogenerated N-centred radicals as a general, catalytic direct hydrogen atom transfer platform for aliphatic C–H functionalization","authors":"Boya Feng \u0000 (, ), Mattia Lepori, Michał Domański, Soňa Boháčová, Daniel Bím, Lucie Ludvíková, Tomáš Slanina, Prakash C. Tiwari, Guodong Zhang \u0000 (, ), Luigi Dolcini, Timothy Noël, Joshua P. Barham","doi":"10.1038/s41929-026-01539-2","DOIUrl":"10.1038/s41929-026-01539-2","url":null,"abstract":"The introduction of diverse functionalities into omnipresent aliphatic C–H bonds is of notable value yet challenging in catalysis. While hydrogen atom transfer has emerged as a premier strategy, existing protocols frequently rely on O-centred radicals either generated from hazardous stoichiometric peroxides or within photocatalysts that are promiscuous in their excited state reactivity and non-conducive to structural tuning around the reactive centre. Here we disclose a general platform of readily prepared 9-arylacridine catalysts—a class of neutral, N-centred photocatalysts—that mediate aliphatic C–H bond hydrogen atom transfer under mild conditions. This strategy enables efficient generation of alkyl radicals, allowing various functionalizations ranging from activated substrates to gaseous ethane. The platform features broad substrate scope, scalability and compatibility with transition metal catalysis as well as multicomponent reactions. Its utility is demonstrated in the streamlined synthesis of pharmaceutical synthons and late-stage functionalization of bioactive molecules. Detailed mechanistic studies highlight the crucial role of ortho-substituents on the 9-aryl moiety of catalysts, providing a rational basis for catalyst design. Direct hydrogen atom transfer (d-HAT) for C(sp3)–H functionalization classically relies on O-centred photocatalysts. Now, neutral N-centred acridine photocatalysts have been added to the toolbox, enabling mild, scalable d-HAT that is compatible with a broad substrate scope and transition metal catalysis.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"676-688"},"PeriodicalIF":48.3,"publicationDate":"2026-06-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01539-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148290924","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The pH-dependant stabilization and interphase coupling of Pd species during alcohol oxidation 醇氧化过程中Pd物质的ph依赖性稳定和相间偶联
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-04 DOI: 10.1038/s41929-026-01547-2
Nouf Ali Alnahdi, Bohyeon Kim, Isaac T. Daniel, Samuel Pattisson, Mark Douthwaite, James Spragg, David J. Morgan, Thomas E. Davies, Alex Stenner, Stuart H. Taylor, Steven McIntosh, Graham J. Hutchings
{"title":"The pH-dependant stabilization and interphase coupling of Pd species during alcohol oxidation","authors":"Nouf Ali Alnahdi, Bohyeon Kim, Isaac T. Daniel, Samuel Pattisson, Mark Douthwaite, James Spragg, David J. Morgan, Thomas E. Davies, Alex Stenner, Stuart H. Taylor, Steven McIntosh, Graham J. Hutchings","doi":"10.1038/s41929-026-01547-2","DOIUrl":"10.1038/s41929-026-01547-2","url":null,"abstract":"Heterogeneous catalysts consistently suffer from the leaching of active components into the fluid phase, causing loss in activity and lifetime. Here we demonstrate, exemplified with the thermocatalytic oxidation of 1,2-propanediol, a metal stabilization mechanism arising from electrochemical coupling of half reactions between physically separated carbon-supported Au and Pd catalysts. When electrochemically coupled, polarization of each metal to an operating mixed potential occurs as a function of the Au:Pd molar ratio that, at pH 9–10, significantly reduces Pd leaching. At pH 14, where this stabilization no longer holds, we clearly show that an active redox mechanism can exist between disparate catalytic species in the liquid and solid phase, and that this leads to the cycling of Pd speciation as well as considerable enhancements in the rate of oxidation. Metal dissolution is a common cause for catalyst deactivation in heterogenous catalysis. Now, after mapping Pd speciation as a function of pH, a cooperative enhancement mechanism between separated Au/C and Pd/C catalysts and involving solid and dissolved Pd species is identified for alcohol oxidation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"609-619"},"PeriodicalIF":48.3,"publicationDate":"2026-06-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01547-2.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336887","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Selective C–C bond cleavage-enabled annulation between β-lactams and π-systems via Ni–Al bimetallic catalysis 通过Ni-Al双金属催化,β-内酰胺和π-体系之间的选择性C-C键裂解使环形成
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-03 DOI: 10.1038/s41929-026-01552-5
Rong-Hua Wang, Wei-Wei Xu, Deng Pan, Yinpeng Wang, Yuzhen Zheng, Cui Yu, Jiang-Fei Li, Tao Zhang, Yi Li, Xiao-Song Xue, Qi-Lin Zhou, Mengchun Ye
{"title":"Selective C–C bond cleavage-enabled annulation between β-lactams and π-systems via Ni–Al bimetallic catalysis","authors":"Rong-Hua Wang, Wei-Wei Xu, Deng Pan, Yinpeng Wang, Yuzhen Zheng, Cui Yu, Jiang-Fei Li, Tao Zhang, Yi Li, Xiao-Song Xue, Qi-Lin Zhou, Mengchun Ye","doi":"10.1038/s41929-026-01552-5","DOIUrl":"10.1038/s41929-026-01552-5","url":null,"abstract":"The substitution of classical dienes with C–C bonds in Diels–Alder-type reactions is a compelling paradigm in modern syntheses. Although activation of C–C bonds α to a single heteroatom has been well established, extending this strategy to synthetically valuable C–C moieties α to two heteroatoms remains challenging because of the competing activation of adjacent C–heteroatom bonds. Here we overcome this limitation through the development of a selective C2–C3 bond activation protocol in β-lactams, which operates with remarkable fidelity despite the presence of the intrinsically more reactive N1–C2 bond. Key to this work is the phosphine oxide-ligating Ni–Al bimetallic catalyst system, which positions nickel at C2–C3, suppresses C–N activation and facilitates annulation with diverse π-systems (alkynes/alkenes). This mechanistically guided strategy affords δ-lactam homologues in up to 99% yield, representing a marked departure from conventional cycloaddition approaches constrained by inherent bond reactivity hierarchies. Selective C–C bond activation adjacent to two heteroatoms is challenging due to competing C–X cleavage. This work develops a Ni–Al catalytic system that enables precise activation of the inert C2–C3 bond in β-lactams, facilitating efficient annulations with π-systems with high regiocontrol.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"645-654"},"PeriodicalIF":48.3,"publicationDate":"2026-06-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336879","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}
引用次数: 0
Conformation-driven C3-C(sp3)–H arylation of saturated azacycles using Pd catalyst Pd催化饱和氮杂环构象驱动的C3-C(sp3) -H基化反应
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-02 DOI: 10.1038/s41929-026-01548-1
Chia-Yu Chen, Zhoulong Fan, Daniel A. Strassfeld, Hau Sun Sam Chan, Miguel Cohen Suarez, Md Emdadul Hoque, Jin-Quan Yu
{"title":"Conformation-driven C3-C(sp3)–H arylation of saturated azacycles using Pd catalyst","authors":"Chia-Yu Chen, Zhoulong Fan, Daniel A. Strassfeld, Hau Sun Sam Chan, Miguel Cohen Suarez, Md Emdadul Hoque, Jin-Quan Yu","doi":"10.1038/s41929-026-01548-1","DOIUrl":"10.1038/s41929-026-01548-1","url":null,"abstract":"Directed Pd-catalysed site-selective C(sp3)–H activation offers an effective route to functionalized amines that are highly valued yet synthetically challenging in drug discovery. Despite the central importance of diverse saturated azacycles in biologically active molecules, a general strategy harnessing native endocyclic nitrogen that only works for specific types of conformation as the directing element for C–H activation of these scaffolds has remained unsolved due to conformational constraints imposed by transannular transition states. Here we report a Pd-catalysed, site- and diastereo-selective C3-C(sp3)–H arylation of saturated azacycles, enabled by temporarily converting the endocyclic nitrogen into an N-oxide directing group and a bifunctional ligand. This one-bond extension strategy enables favourable five-membered cyclopalladation, with axial N-oxide orientation being crucial for overcoming transannular ring strain as to reach the syn-axial C3-C(sp3)–H bond. The C–H activation of secondary and tertiary amines under directed Pd(II) catalysis remains challenging. Now the authors report a Pd-catalysed, site- and diastereoselective C3-C(sp3)–H arylation of saturated azacycles, enabled by conversion of the endocyclic nitrogen as N-oxide directing group and a bifunctional ligand.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"620-629"},"PeriodicalIF":48.3,"publicationDate":"2026-06-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.nature.comhttps://www.nature.com/articles/s41929-026-01548-1.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336878","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The kinetic basis of bifunctional OX–ZEO catalysts for syngas conversion to light olefins 合成气转化为轻烯烃的双功能OX-ZEO催化剂的动力学基础
IF 48.3 1区 化学
Nature Catalysis Pub Date : 2026-06-01 DOI: 10.1038/s41929-026-01546-3
Zhuangzhuang Lai, Danfeng Xiong, Peijun Hu, Jianfu Chen, Haifeng Wang
{"title":"The kinetic basis of bifunctional OX–ZEO catalysts for syngas conversion to light olefins","authors":"Zhuangzhuang Lai, Danfeng Xiong, Peijun Hu, Jianfu Chen, Haifeng Wang","doi":"10.1038/s41929-026-01546-3","DOIUrl":"10.1038/s41929-026-01546-3","url":null,"abstract":"Despite considerable progress in oxide–zeolite (OX–ZEO) bifunctional catalysts for ketene-mediated syngas conversion, the origin of inter-component synergy and its dependence on spatial proximity remain unclear. Here we develop a diffusion-bridged, two-component microkinetic model that incorporates the entire reaction network over the ZnCrOx/mordenite (MOR) catalyst. The model captures the coupled reaction–diffusion dynamics and quantitatively elucidates the synergetic mechanism underlying selective syngas-to-light-olefin conversion. We show that MOR enhances light-olefin selectivity by overcoming the thermodynamic limitation of CH2CO formation on the oxide via a more favourable pathway. Furthermore, the model predicts an inverted U-shaped dependence of light-olefin selectivity with proximity, arising from a balance between intermediate transfer and Zn migration, the latter generating [ZnOH]+ species that promote undesired hydrogenation. More broadly, we establish a general reaction–diffusion coupling kinetic framework that quantifies the optimal combination principles for OX–ZEO systems. The predictions agree well with experimental observations and provide guidance for designing high-performance bifunctional catalysts. Bifunctional oxide–zeolite catalysts work in tandem to produce light olefins from syngas, but the precise mechanistic picture is complex and remains elusive. Now the reaction mechanism on a ZnCrOx/mordenite catalyst is studied in detail using a diffusion-bridged microkinetic model, and design principles are proposed.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 6","pages":"598-608"},"PeriodicalIF":48.3,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148336877","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}
引用次数: 0
Dynamic clusters unlock propane dehydrogenation 动态集群解锁丙烷脱氢
IF 44.6 1区 化学
Nature Catalysis Pub Date : 2026-05-28 DOI: 10.1038/s41929-026-01540-9
Anna Clara Noguti, Francine Bertella, Christian Wittee Lopes
{"title":"Dynamic clusters unlock propane dehydrogenation","authors":"Anna Clara Noguti, Francine Bertella, Christian Wittee Lopes","doi":"10.1038/s41929-026-01540-9","DOIUrl":"10.1038/s41929-026-01540-9","url":null,"abstract":"Propylene production from propane faces persistent catalytic limitations. Now, an unusual form of subnanometre platinum–tin clusters confined within zeolite pores overcome the long-standing productivity–stability trade-off in propane dehydrogenation.","PeriodicalId":18845,"journal":{"name":"Nature Catalysis","volume":"9 5","pages":"485-486"},"PeriodicalIF":44.6,"publicationDate":"2026-05-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148040017","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}
引用次数: 0
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