Journal of Catalysis最新文献_第4页

Unraveling the evolution of oxygen species and its role in adjusting catalytic performance over LaAlO3-based catalysts in oxidative coupling of methane 揭示了甲烷氧化偶联中氧的演化及其在laalo3基催化剂上调节催化性能的作用

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-12 DOI: 10.1016/j.jcat.2026.116695

Yaqian Zhang , Xingxu Wang , Bingying Han , Lixia Ling , Baojun Wang , Maohong Fan , Riguang Zhang

{"title":"Unraveling the evolution of oxygen species and its role in adjusting catalytic performance over LaAlO3-based catalysts in oxidative coupling of methane","authors":"Yaqian Zhang , Xingxu Wang , Bingying Han , Lixia Ling , Baojun Wang , Maohong Fan , Riguang Zhang","doi":"10.1016/j.jcat.2026.116695","DOIUrl":"10.1016/j.jcat.2026.116695","url":null,"abstract":"<div><div>The oxidative coupling of methane (OCM) reaction is hindered by fundamental scientific challenges including the difficulty in CH<sub>4</sub> activation and the inability to inhibit deep oxidation. In this study, the LaAlO<sub>3</sub> catalyst, which exhibits excellent low-temperature activity and thermal stability, was selected. The structure–activity relationship among the catalyst surface structure, surface oxygen species, and reaction performance was systematically explored using DFT calculations and microkinetic modeling. The results indicate that different surface terminations (LaO- and AlO<sub>2</sub>-terminations) of LaAlO<sub>3</sub> catalyst exhibit distinct oxygen species. The evolution pathway of oxygen species on the LaO-termination surface proceeds as O<sup>2–</sup>→O<sub>2</sub><sup>–</sup>→O<sub>2</sub><sup>2–</sup>→O<sup>2–</sup>, while on the AlO<sub>2</sub>-termination surface it follows O<sup>2–</sup>→O<sub>2</sub><sup>2–</sup>→O<sup>2–</sup>. Among these oxygen species, O<sup>2–</sup> plays a dominant role in CH<sub>4</sub> dissociation. The LaO-termination demonstrates three major advantages: higher CH<sub>4</sub> dissociation activity, superior C<sub>2</sub>H<sub>4</sub> production activity, and enhanced selectivity, establishing it as the dominant active termination. Doping the LaO-termination catalysts with alkaline earth metals (Mg, Ca, Sr) do not alter the types of oxygen species but significantly modulate reaction characteristics. Bader charge of surface O<sup>2–</sup> serves as an effective descriptor for predicting CH<sub>4</sub> dissociation capability of M/LaO-p-O<sup>2–</sup> catalysts. Under realistic conditions, due to fewer surface free sites, Ca/LaO-p-O<sup>2–</sup> exhibits a lower C<sub>2</sub>H<sub>4</sub> formation rate than Sr/LaO-p-O<sup>2–</sup>.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116695"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145956885","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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A tandem visible-light/heterogeneous-alumina catalytic platform for sustainable transition-metal-free cyclobutene synthesis 可见光/多相氧化铝串联催化平台可持续合成无过渡金属环丁烯

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-27 DOI: 10.1016/j.jcat.2026.116726

Zhe Wang , Jie Huang , Min Zhou, Lin Ma, Min Zhang

引用次数: 0

Corrigendum to “Robust rGO-supported α-FeOOH/Fe2O3 nanorods catalyst: Unveiling the role of χ-Fe5C2 phase and rGO for exceptional stability in Fischer–Tropsch synthesis”. [J. Catal. 453 (2026) 116584] “稳健的rGO负载α-FeOOH/Fe2O3纳米棒催化剂：揭示χ-Fe5C2相和rGO在费托合成中特殊稳定性的作用”的勘误。[J。Catal. 453 (2026) 116584]

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-07 DOI: 10.1016/j.jcat.2025.116666

Juan Zhang , Mohamed Abbas , Weibin Fan , Jiangang Chen

引用次数: 0

Structural transformation promoted oxygen vacancy creation and spatial separation of vacancies and holes in bismuth molybdate boost photocatalytic nitrogen fixation and stability 钼酸铋的结构转变促进了氧空位的产生，空位和空穴的空间分离促进了光催化固氮和稳定性

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-16 DOI: 10.1016/j.jcat.2026.116698

Zhenke Fan , Haiping Li , Kai Gao , Quanhua Deng , Yuguo Xia , Shu Liu , Yunbo Zang , Wanguo Hou

{"title":"Structural transformation promoted oxygen vacancy creation and spatial separation of vacancies and holes in bismuth molybdate boost photocatalytic nitrogen fixation and stability","authors":"Zhenke Fan , Haiping Li , Kai Gao , Quanhua Deng , Yuguo Xia , Shu Liu , Yunbo Zang , Wanguo Hou","doi":"10.1016/j.jcat.2026.116698","DOIUrl":"10.1016/j.jcat.2026.116698","url":null,"abstract":"<div><div>Oxygen vacancy (Ov)-containing semiconductors hold great promise for photocatalytic nitrogen fixation, as Ovs serve as efficient N<sub>2</sub> activation centers. However, the low photocatalytic stability of Ovs has often been overlooked, and few strategies have been explored to enhance their stability. Moreover, methods to effectively create Ovs are still under investigation. Herein, crystalline structure transformation from BiOBr microplates to hierarchical Bi<sub>2</sub>MoO<sub>6</sub> microplates consisting of sharp-end nanobelts was found to facilitate creation of Ovs in Bi<sub>2</sub>MoO<sub>6</sub> during mannitol reduction. The Ov-containing Bi<sub>2</sub>MoO<sub>6</sub> (Ov-BMO) exhibits improved photocatalytic nitrogen fixation activity but low stability in pure water. To enhance the stability and activity, the Ov-BMO/α-Co(OH)<sub>2</sub> heterojunction was constructed to spatially separate Ovs and photogenerated holes and exhibits a solar-to-chemical conversion efficiency of 0.1% and an apparent quantum yield of 4.6% at 420 nm, which are among the top of the reported values. This work offers effective strategies for creating and stabilizing Ovs in Bi<sub>2</sub>MoO<sub>6</sub> to boost photocatalytic nitrogen fixation.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116698"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995785","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

Stable and efficient bifunctional cobalt-based phosphides for industrial-current water splitting: From multi-strategy engineering to mechanistic insights 稳定和高效的双功能钴基磷化物用于工业水流分解：从多策略工程到机械洞察

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-16 DOI: 10.1016/j.jcat.2026.116703

Haiyu Yao , Heng Zhang , Xuerong Shi, Shengming Zhang, Min Zhu, Haichao Xiong, Shusheng Xu

{"title":"Stable and efficient bifunctional cobalt-based phosphides for industrial-current water splitting: From multi-strategy engineering to mechanistic insights","authors":"Haiyu Yao , Heng Zhang , Xuerong Shi, Shengming Zhang, Min Zhu, Haichao Xiong, Shusheng Xu","doi":"10.1016/j.jcat.2026.116703","DOIUrl":"10.1016/j.jcat.2026.116703","url":null,"abstract":"<div><div>In the context of industrial-current density water electrolysis, material stability and catalytic activity remain critical challenges. Herein, a CoFeP/NF electrocatalyst enabled by pre-activation, hierarchical nanosheet architecture, bimetallic synergy, and carbon protection demonstrates good bifunctional OER/HER performance. The optimal CoFeP/NF requires overpotentials of 235 and 440 mV to achieve current densities of 10 and 2000 mA cm<sup>−2</sup> for alkaline OER, respectively. In line with density-functional theory predictions, the CoFeP/NF also exhibits high alkaline HER activity, demanding an overpotential of 79 mV to reach 10 mA cm<sup>−2</sup>. The assembled CoFeP/NF||CoFeP/NF electrolyzer maintains stable operation for 1100 h at ∼200 mA cm<sup>−2</sup>. The comprehensive mechanism, encompassing the pre-activation mechanism, reaction kinetics, and origin of stability, has been meticulously investigated via the combination of theoretical calculations and in/ex-situ experimental characterizations. The findings offer a universal strategy for the rational design of efficient electrocatalysts for industrial-current–density water splitting.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116703"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145993300","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

Xantphos-derived porous polymer: a robust solid-state ligand for efficient Pd-catalyzed alkoxycarbonylation of alkenes from mono-alcohols to polyols 黄磷衍生的多孔聚合物：一种强大的固体配体，用于高效的pd催化烯烃从单醇到多元醇的烷氧羰基化

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-06 DOI: 10.1016/j.jcat.2026.116677

Yuyong Zhang , Yuanjun Zhao , Yuanyuan Zhu , Yudi Wu , Zhaozhan Wang , Jinglin Mu , Yong Yang

{"title":"Xantphos-derived porous polymer: a robust solid-state ligand for efficient Pd-catalyzed alkoxycarbonylation of alkenes from mono-alcohols to polyols","authors":"Yuyong Zhang , Yuanjun Zhao , Yuanyuan Zhu , Yudi Wu , Zhaozhan Wang , Jinglin Mu , Yong Yang","doi":"10.1016/j.jcat.2026.116677","DOIUrl":"10.1016/j.jcat.2026.116677","url":null,"abstract":"<div><div>The integration of superior homogeneous catalytic activity with the practical advantages of facile separation and robust recyclability of heterogeneous systems remains a grand challenge. Here, we report a heterogenized bidentate phosphine ligand, constructed by integrating commercial Xantphos into a hypercrosslinked porous polymer, as a versatile platform for Pd-catalyzed alkoxycarbonylation. The tailored polymer, featuring a high surface area, hierarchical pores, and chemical robustness, provides privileged coordination microenvironments. It empowers highly efficient alkoxycarbonylation of diverse alkenes with various alcohols, including monoalcohols, diols, and polyols, to produce valuable esters with activity and selectivity comparable to its homogeneous molecular counterpart. Moreover, the catalytic system enables the in-situ formation of a robust Pd catalyst, wherein Pd nanoparticles are stabilized and uniformly dispersed via strong Pd-P coordination. This resulting catalyst demonstrates exceptional durability, being readily recycled over ten times without significant degradation in performance. This work pioneers a versatile platform for ligand immobilization that effectively bridges homogeneous efficiency with heterogeneous durability, unlocking efficient and sustainable pathways for carbonylation and other ligand-mediate transformations.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116677"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145924007","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

BEA zeolite encapsulated defective Co sites for solvent- and additive-free N-alkylation of amines with aromatic alcohols BEA沸石包覆有缺陷的Co位点，用于无溶剂和无添加剂的胺与芳香醇的n -烷基化

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-23 DOI: 10.1016/j.jcat.2026.116713

Meng Xu , Zhongliang Tang , Yue Wu , Menglin Xie , Biao Meng , Xiao Chi , Xiaojiang Yu , Xiaoling Liu , Shibo Xi , Yu Zhou , Jun Wang

{"title":"BEA zeolite encapsulated defective Co sites for solvent- and additive-free N-alkylation of amines with aromatic alcohols","authors":"Meng Xu , Zhongliang Tang , Yue Wu , Menglin Xie , Biao Meng , Xiao Chi , Xiaojiang Yu , Xiaoling Liu , Shibo Xi , Yu Zhou , Jun Wang","doi":"10.1016/j.jcat.2026.116713","DOIUrl":"10.1016/j.jcat.2026.116713","url":null,"abstract":"<div><div>Hydrogen borrowing amination provides a sustainable alcohol-based N-alkylation method for the amine synthesis and functionalization, yet the development of non-noble metal catalysts that are effective under additive- and solvent-free conditions remains a huge challenge. Herein, we report a Cobalt (Co)-containing zeolite, Co@Beta, prepared by directly encapsulating defect Co sites within BEA framework <em>via</em> an acid co-hydrolysis route. Co@Beta shows excellent catalytic performance in the N-alkylation of benzyl alcohol with aniline, achieving > 92% yield and a turnover frequency (TOF) of 466 h<sup>−1</sup> without external solvent or additive. The catalyst is stable during the recycling amination and extendable to the amination between various aromatic alcohols and amines. <em>In situ</em> spectroscopic analysis, theoretical calculations, as well as step-by-step comparison with post-loaded analogues, reveal that defect Co sites within Co@Beta are active centers, thereby lowering the energy barrier for the rate-determining dehydrogenation step and underpinning the superior amination performance.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116713"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033865","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

Understanding metal-support interaction for single-walled carbon nanotube synthesis: a comparative study of Co on MgO and Al2O3 了解单壁碳纳米管合成中金属-载体相互作用：Co对MgO和Al2O3的比较研究

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-27 DOI: 10.1016/j.jcat.2026.116722

Jiwoo Kim , Dong Hwan Kim , Seungki Hong , Tae Hoon Seo , Jaegeun Lee

{"title":"Understanding metal-support interaction for single-walled carbon nanotube synthesis: a comparative study of Co on MgO and Al2O3","authors":"Jiwoo Kim , Dong Hwan Kim , Seungki Hong , Tae Hoon Seo , Jaegeun Lee","doi":"10.1016/j.jcat.2026.116722","DOIUrl":"10.1016/j.jcat.2026.116722","url":null,"abstract":"<div><div>As the demand for precisely tailored carbon nanotube (CNT) properties increases, catalyst design becomes increasingly important. In the field of catalysis, metal–support interaction (MSI) has been recognized as a key strategy for tuning catalyst performance. To better understand how MSI affects CNT synthesis, this study investigates cobalt-based catalysts supported on Al<sub>2</sub>O<sub>3</sub> and MgO. CNTs synthesized using the Co/MgO exhibited higher crystallinity and broader diameter distribution than those synthesized using Co/Al<sub>2</sub>O<sub>3</sub>. Detailed characterization—including X-ray analyses, transmission electron microscopy, and temperature-programmed reduction—revealed that both catalysts exhibited MSI accompanied by compositional reconstruction, but through different mechanisms: Co/Al<sub>2</sub>O<sub>3</sub> formed compounds, while Co/MgO developed solid solutions. Based on these findings, we proposed distinct mechanisms of metal nanoparticle formation to explain the different interphase formation behavior observed in the two catalyst systems. Utilizing this hypothesis, formation of solid solution in the Co/MgO catalyst was regulated by adjusting the calcination temperature, and enhanced solid solution formation promoted preferential growth of single-walled CNTs (SWCNTs) under specific conditions. Under these optimized Co/MgO conditions, the CNT product achieved ∼10% carbon yield, an <em>I</em><sub>G</sub>/<em>I</em><sub>D</sub> ratio of 4.5 ± 1.1, a TGA decomposition peak at 531.87 °C indicating high thermal stability, and facile purification leaving only 1.5% residual mass. Overall, this work highlights how different types of MSI—compound formation versus solid solution formation—can lead to fundamentally distinct CNT growth behaviors, providing new insights for the rational design of catalysts for SWCNT production.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116722"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072539","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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Theoretical investigation of decomposition and hydrolysis of sulfonamides on CeO2(111) 磺胺类化合物在CeO2（111）上分解水解的理论研究

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2025-12-31 DOI: 10.1016/j.jcat.2025.116663

Ye Xu , Timm McNeese

引用次数: 0

Prediction on origin of chemoselectivity for N-Heterocyclic carbene (NHC)-catalyzed radical relay reactions n -杂环碳（NHC）催化自由基接力反应的化学选择性来源预测

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-16 DOI: 10.1016/j.jcat.2026.116702

Qianqian Shi , Keke He , Zhile Dang , Jing Zhang , Donghui Wei , Yu Lan

{"title":"Prediction on origin of chemoselectivity for N-Heterocyclic carbene (NHC)-catalyzed radical relay reactions","authors":"Qianqian Shi , Keke He , Zhile Dang , Jing Zhang , Donghui Wei , Yu Lan","doi":"10.1016/j.jcat.2026.116702","DOIUrl":"10.1016/j.jcat.2026.116702","url":null,"abstract":"<div><div>Discovering new radical generation mechanism and understanding origin of chemoselectivity of transformation reactions between the highly active radicals have been and continue to be the hot topics in radical chemistry. Different from the generally proposed single-electron transfer (SET) mechanism, the electron transfer along bond transformation (ETBT) mechanism has been suggested to be also possible and general for the radical reactions. To confirm this issue, the possible ETBT mechanisms and the theoretical method for chemoselectivity prediction of N-heterocyclic carbene (NHC)-catalyzed radical relay reactions have been systematically investigated by performing density functional theory (DFT) calculations. Herein, origin of chemoselectivity for these kinds of reactions has been explored by the distortion energy analysis, and a good linear relationship between the distortion energy (Δ<em>E</em><sub>dist</sub><sup>‡</sup>) and spin population change (Δ<em>e</em>) of the radical species has been discovered for the first time. Furthermore, the Fukui function vector index has been successfully employed to predict chemical selectivity in radical relay reactions.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"455 ","pages":"Article 116702"},"PeriodicalIF":6.5,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995784","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