Journal of Catalysis最新文献

{"title":"Advancing electrocatalyst discovery through the lens of data science: State of the art and perspectives","authors":"Xue Jia ,&nbsp;Tianyi Wang ,&nbsp;Di Zhang ,&nbsp;Xuan Wang ,&nbsp;Heng Liu ,&nbsp;Liang Zhang ,&nbsp;Hao Li","doi":"10.1016/j.jcat.2025.116162","DOIUrl":"10.1016/j.jcat.2025.116162","url":null,"abstract":"<div><div>The integration of data science into electrocatalysis has revolutionized the discovery of high-performance catalysts for sustainable energy applications. To emphasize the role of data science and guide future research in electrocatalyst design, this mini-review traces the evolution from low-dimensional data science—rooted in density functional theory (DFT) descriptors such as <em>d</em>-band center and binding/adsorption energies—to high-dimensional analytics powered by large-scale computational datasets and machine learning (ML). First, DFT-derived parameters establish predictive volcano models for various electrochemical reactions, linking atomic-scale descriptors to macroscopic performance within the framework of low-dimensional data science. Meanwhile, with the development of large-scale datasets, ML deciphers complex structure–property relationships, accelerating the design of promising electrocatalysts. Additionally, machine learning potentials (MLPs) bridge quantum precision and scalability, not only accelerating thermodynamic adsorption energy calculations but also enabling simulations of dynamic catalytic mechanisms more efficiently. Finally, we discuss emerging opportunities to deepen data science’s impact. This mini-review highlights the transformative role of data science in bridging theoretical insights, computational efficiency, and experimental validation, ultimately accelerating the design of next-generation electrocatalysts for a sustainable energy future.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116162"},"PeriodicalIF":6.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858092","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}

{"title":"An efficient catalyst from electrochemical self-reconstruction of NiFePBA/Ni(OH)2 for 5-hydroxymethylfurfural electrooxidation to produce high-valued 2,5-furandicarboxylic acid","authors":"Xuhui Chen ,&nbsp;Hao Liu ,&nbsp;Lei Chen ,&nbsp;Wei Xiong ,&nbsp;Yuqi Liu ,&nbsp;Xiujuan Sun ,&nbsp;Fang Hao","doi":"10.1016/j.jcat.2025.116159","DOIUrl":"10.1016/j.jcat.2025.116159","url":null,"abstract":"<div><div>The utilization of sustainable lignocellulosic biomass for the production of high-value products could potentially solve the intensive reliance on fossil fuels. 2,5-furandicarboxylic acid (FDCA), obtained from 5-hydroxymethylfurfural (HMF) oxidation, is a significant precursor for biomass converted high-value chemicals. Nowadays, the rational design of pre-catalysts <em>via</em> electrochemical self-reconstruction provides an opportunity to design efficient catalysts for electrooxidation process. In this study, we developed a pre-catalyst consisting of nanoscale cubic NiFePBA anchored on Ni(OH)₂. After electrochemical reconstruction, it demonstrated superior HMF oxidation reaction (HMFOR) performance. The results demonstrate that the electrochemical self-reconstruction process converts nanoscale cubic NiFePBA into nanosheeted metal oxyhydroxide, resulting in the formation of an oxygen defect-rich heterostructure with Ni(OH)₂. This reconstruction process also enhance the electrochemically active surface area, thereby increasing the number of active sites. The combined effect of increased active sites and oxygen defects significantly enhances the HMF adsorption and the HMFOR activity. <em>In situ</em> electrochemical impedance spectroscopy further reveals that the reconstructed NiFePBA/Ni(OH)₂-R exhibits accelerated reaction kinetics and reduced reaction potential during the electrocatalytic oxidation of HMF. The NiFePBA/Ni(OH)₂-R catalyst exhibited exceptional electrochemical performance, achieving a high current density of 50 mA·cm^–2 at a relatively low potential of 1.43 V vs. RHE. This performance is characterized by a remarkable 99.1 % conversion of HMF, 98.5 % selectivity for FDCA, and a Faradaic efficiency of 94.2 %. This study offers valuable insights for the development of high-performance HMFOR electrocatalysts.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116159"},"PeriodicalIF":6.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858130","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}

{"title":"Computational insights into the photocatalytic conversion of CO2 to C2H4 on synergistic dual sites in tandem rhenium-bipyridine/copper-porphyrinic system","authors":"Debo Ding,&nbsp;Xiahe Chen,&nbsp;Hongli Wu,&nbsp;Hai-Min Shen,&nbsp;Teng-Shuo Zhang,&nbsp;Keke Wang,&nbsp;Yun-Fang Yang,&nbsp;Yuan-Bin She","doi":"10.1016/j.jcat.2025.116144","DOIUrl":"10.1016/j.jcat.2025.116144","url":null,"abstract":"<div><div>The rhenium(I)-bipyridine complex (Re-bpy) has been reported to be a very active photocatalyst to stabilize the *CO species in CO₂ reduction, and the copper-porphyrinic triazine framework Cu-PTF was found to be a very good relay partner and cooperator in facilitating the C−C coupling process to generate C₂H₄. To unravel the mechanism of reduction of CO₂ to C₁ and C₂ products and how such two catalysts synergistically promote C−C coupling, we conducted density functional theory (DFT) calculations. The most favorable mechanism comprises the following key steps: CO₂ activation by Re-bpy, formation of Re−CO species, proton-coupled electron transfer (PCET) to form Re−CHO species, synergistic coupling between Re−CHO and Cu−CO to form Cu−CO−CHO−Re intermediate, the PCET to form resting state Cu−CHO−CH₂−Re intermediate, another PCET to generate Cu−CHOH−CH₂−Re, PCET and elimination of H₂O and dissociation to yield C₂H₄. Our DFT calculations provides insights into the catalytic pathways and the cooperative interactions between the two catalysts, paving the way for the development of more efficient catalytic systems for CO₂ reduction reactions.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116144"},"PeriodicalIF":6.5,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853588","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}

{"title":"Enhancing electron penetration through carbon shell of encapsulated catalysts by Co alloying for aromatic nitrobenzene hydrogenation","authors":"Wei He,&nbsp;Yanni Li,&nbsp;Qiuyuan Xiang,&nbsp;Xiyuan Zhang,&nbsp;Jiaxin Yu,&nbsp;Chaofan Ma,&nbsp;Yongyue Yao,&nbsp;Chunyu Yin,&nbsp;Yi Liu,&nbsp;Yebin Zhou,&nbsp;Xiaonian Li,&nbsp;Chunshan Lu","doi":"10.1016/j.jcat.2025.116150","DOIUrl":"10.1016/j.jcat.2025.116150","url":null,"abstract":"<div><div>Encapsulated catalysts have become a new strategy for catalysis in harsh reaction environments due to their unique structural and functional reorganization properties, and they have been widely applied in fields such as electrocatalysis, photocatalysis, and thermocatalysis. In strategies involving encapsulated catalysts, the optimization of electronic properties on the carbon layer surface to enhance reactivity while maintaining adequate encapsulation poses a challenge due to the trade-off between stability, poison resistance, and acid resistance against the performance of metal nanoparticles. Herein, an alloying strategy for Co-Ni bimetal was proposed, which achieves a delicate balance between catalyst activity and stability. Ni plays a pivotal role in promoting the formation of graphitized carbon and the construction of an effective encapsulation structure, thereby ensuring the stability of the catalyst. Co incorporation and alloying with Ni modulates the electronic state and D-band structure within the metallic core, effectively breaking the electronic cloud segregation barrier imposed by the carbon shell. This modulation notably enhances the efficiency of reactions. For the hydrogenation of <em>p</em>-CNB to <em>p</em>-CAN, Co₂Ni₈@C exhibits an extremely low apparent activation energy (53.40 KJ/mol), as well as &gt; 99 % conversion and selectivity.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116150"},"PeriodicalIF":6.5,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853863","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}

{"title":"Selective conversion of ethane to value added products on RhO2(1 1 0): A DFT and microkinetic simulation study","authors":"Seongjun Lee ,&nbsp;Jungwon Yun ,&nbsp;Dasol Bae ,&nbsp;Dohyeon Kim ,&nbsp;Sung Bong Kang ,&nbsp;Dohyung Kang ,&nbsp;Minkyu Kim","doi":"10.1016/j.jcat.2025.116146","DOIUrl":"10.1016/j.jcat.2025.116146","url":null,"abstract":"<div><div>The selective conversion of small alkanes into value-added products presents a significant challenge in catalysis due to the strong tendency toward complete oxidation. In this study, we employed DFT calculations and TPRS simulations to investigate ethane oxidation on the RhO₂(1<!--> <!-->1<!--> <!-->0) surface. Our results demonstrate that the moderate reactivity of RhO₂(1<!--> <!-->1<!--> <!-->0) enhances selectivity for ethylene production, positioning RhO₂(1<!--> <!-->1<!--> <!-->0) as a promising catalyst for the selective oxidation of small alkanes and improved yields of value-added products. Extending beyond RhO₂, we propose that highly reactive transition metal oxide surfaces may exhibit similar C₂H₄ desorption mechanisms involving C₂H₄ reformation-based desorption, as supported by comparisons with highly active IrO₂. This insight suggests that catalytic strategies designed to facilitate reverse reactions for C₂H₄ reformation hold potential for boosting C₂H₄(g) production from C₂H₆ oxidation on active transition metal oxides.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"448 ","pages":"Article 116146"},"PeriodicalIF":6.5,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853867","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}

{"title":"Hierarchical hollow silicalite encapsulated Cu-Fe oxides for selectively oxidative depolymerization of lignin to diethyl meleate","authors":"Lixia Li ,&nbsp;Juanhua Kong ,&nbsp;Jinxing Long ,&nbsp;Zhengping Cai ,&nbsp;Qiang Zeng ,&nbsp;Kejia Wu ,&nbsp;Yingying Zhan ,&nbsp;Sijie Liu ,&nbsp;Hongyan He ,&nbsp;Xuehui Li","doi":"10.1016/j.jcat.2025.116157","DOIUrl":"10.1016/j.jcat.2025.116157","url":null,"abstract":"<div><div>Heterogeneously catalytic depolymerization of lignin into value-added biochemicals are imperative, yet challengeable by the limited mass transport of lignin and the non-ideal spatial distributions of active sites in catalysts. Herein, a series of polycrystalline materials with Cu and Fe oxides encapsulated in hierarchical hollow nano silicalite (Cu<em>_x</em>-Fe<em>_y</em>@HhNS) were designed for step-by-step oxidative conversion of lignin into diethyl meleate (DEM). 92.0 % conversion of lignin with an exceptional DEM yield of 31.2 wt% and selectivity of 70.7 % was achieved at 150 °C for 24 h using Cu_2.5-Fe_2.2@HhNS. A series of controlled experiments and characterization showed clearly that the superior performance in DEM production was attributed to the enhanced tandem processes of lignin C<em>_α</em>-C<em>_β</em> bonds deconstruction by framework Cu²⁺, subsequently aromatic ring-cleavage by the isolated framework Fe³⁺, and the well-balanced micro-/mesoporosity ratio of Cu<em>_x</em>-Fe<em>_y</em>@HhNS facilitates the diffusion of lignin macromolecules/products, contributing to the excellent DEM yield and selectivity as well. Further mechanistic investigation illustrated that the process proceeds <em>via</em> a single electron transfer pathway. Consequently, this work provides new insights into lignin valorization to bulk chemicals, paving the way for biomass-derived recyclable polymeric materials as sustainable alternative to traditional petroleum-based routes.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"448 ","pages":"Article 116157"},"PeriodicalIF":6.5,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849888","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}

{"title":"Unparalleled dimerization of trans-2-butene to 3,4-dimethyl-1-hexene on iron-based catalyst","authors":"Kang Gao ,&nbsp;Guangjing Feng ,&nbsp;Chaoan Liang ,&nbsp;Zhuang Wang ,&nbsp;Xiaoyan Sun ,&nbsp;Jianhua Liu ,&nbsp;Chungu Xia ,&nbsp;Yuxiao Ding","doi":"10.1016/j.jcat.2025.116155","DOIUrl":"10.1016/j.jcat.2025.116155","url":null,"abstract":"<div><div><em>Trans</em>-2-butene is regularly burned as a liquefied petroleum gas (LPG) component in several developing countries due to its inertness and inseparability in comparison to other butene isomers (1-butene and isobutene), resulting in low-value utilization of resource and environmental degradation. The generation of high-carbon olefins via <em>trans</em>-2-butene oligomerization has become one of the most effective ways for its high-value valorization. Octene is currently undersupplied via ethylene oligomerization, and its traditional crafts are costly due to separation from full-fraction α-olefins (C₄-C₃₀). In the present work, we synthesized a series of novel 2-phenyl-ketimine-1,10-phenanthroline iron complexes (Fe0-Fe9). Fe2 catalyst realizes the dimerization of <em>trans</em>-2-butene through homogeneous catalysis at moderate conditions (0.2 MPa, 30 °C), obtaining 3,4-dimethyl-1-hexene with 99.9 % selectivity. In contrast to the reported heterogeneous catalysts, our catalytic system exhibits a considerable improvement in activity and selectivity.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116155"},"PeriodicalIF":6.5,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849887","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}

{"title":"Cobalt-catalyzed esterification of organohalides with carbon monoxide","authors":"Heng Yang,&nbsp;Yan Jiao,&nbsp;Guodong Zhang,&nbsp;Pan Gao,&nbsp;Feng Chen","doi":"10.1016/j.jcat.2025.116154","DOIUrl":"10.1016/j.jcat.2025.116154","url":null,"abstract":"<div><div>Esters are fundamental compounds in materials science, medicinal chemistry, and organic synthesis. Numerous synthetic methods have been developed to construct ester functional groups. The transition metal-catalyzed carbonylation of aryl halides with alcohols is well-established, with palladium catalysts being the most commonly used. However, the development of non-noble metal-based catalysts for carbonylation reactions has become attractive due to their cost-effectiveness. In this study, we report a novel homogeneous cobalt-catalyzed system for the carbonylation of aryl bromides and aryl chlorides with alkyl halides directly. Notably, this methodology efficiently prepares specialized esters using inexpensive alkyl halides, offering a more economical alternative to using the corresponding alcohols.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116154"},"PeriodicalIF":6.5,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143849886","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}

{"title":"Carbon nanotube-supported Co-N-C with enriched mesopores for hydrogenation of nitro compounds","authors":"Chongqing Wang ,&nbsp;Jianfei Dang ,&nbsp;Yajing Han ,&nbsp;Qinggan Zeng ,&nbsp;Liqiang Wang","doi":"10.1016/j.jcat.2025.116152","DOIUrl":"10.1016/j.jcat.2025.116152","url":null,"abstract":"<div><div>Developing noble metal-free catalysts that enable hydrogenation reduction of nitro compounds to perform under mild conditions is highly attractive yet remains a significant challenge. Herein, carbon nanotube-supported Co-N-C with abundant mesopores (Co₁/CoNPs@CNT) was synthesized via in situ pyrolysis of zeolitic imidazolate framework-67 encapsulated ZnO (ZnO@ZIF-67) for catalytic hydrogenation. The Co₁/CoNPs@CNT catalyst features abundant atomically dispersed CoNx active sites that are easily accessible to substrates. Additionally, theoretical calculations suggest CoNx on curved surfaces favours the H₂ dissociation and the second N<img>O bond breaking (PhNOH* + H* → PhN* + H₂O) more than that on flat surfaces, two crucial steps in the hydrogenation of nitro compounds. As a result, Co₁/CoNPs@CNT exhibits outstanding catalytic performance, enabling the hydrogenation reaction to go smoothly under mild conditions (50 °C, 1 bar H₂) with high conversion and selectivity across a range of substrates.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116152"},"PeriodicalIF":6.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143847021","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}

{"title":"Propane dehydroaromatization on Ga-modified HZSM-5 catalyst: Brønsted/Lewis acid synergistic effect","authors":"Hui Zhang ,&nbsp;Jing Wang ,&nbsp;Caiping Ma ,&nbsp;Riguang Zhang ,&nbsp;Baojun Wang ,&nbsp;Yang Zhang ,&nbsp;Xiaofeng Li ,&nbsp;Lixia Ling","doi":"10.1016/j.jcat.2025.116147","DOIUrl":"10.1016/j.jcat.2025.116147","url":null,"abstract":"<div><div>The HZSM-5 catalyst modified with Ga species exhibits excellent reaction performance for propane dehydroaromatization, a process that involves propane dehydrogenation to propylene, and further formation of aromatics via polymerization, cyclization, dehydrogenation, etc. The detailed mechanism of the synergistic effect between Ga species and Brønsted acid with each other during propane dehydroaromatization remains unclear due to the complexity and extreme branching of aromatization reaction pathways. In this study, the complete reaction process for propane dehydroaromatization on Ga-modified HZSM-5 is investigated based on the density functional theory (DFT) method. The results indicate that the Ga-modified HZSM-5 catalysts with [GaH]²⁺ species at all studied sites show superior thermodynamic and kinetic stability, with only [GaH]²⁺ species at the T3-T11 and T3-T5 sites exhibiting excellent dehydrogenation performance. In propane dehydroaromatization, the dehydrogenation reactions dominated by [GaH]²⁺ species tend to occur on the framework O atom surrounding [GaH]²⁺ species with stronger Lewis base strength, while polymerization and cyclization reactions dominated by Brønsted acid tend to occur on Brønsted acid with stronger acid strength. The synergistic effect between [GaH]²⁺ species and Brønsted acid is reflected in the fact that the [GaH]²⁺ species can indirectly improve the activity of propylene polymerization and C6 diene cyclization reactions on the Brønsted acid by enhancing the Brønsted acid strength, and in turn, the Brønsted acid enables the [GaH]²⁺ species to exist more stably kinetically by promoting the conversion of [GaH₂]⁺ species to [GaH]²⁺ species. This study contributes to the enriched understanding of the Brønsted/Lewis acid synergistic effect and the role of acidity-basicity during propane dehydroaromatization on Ga-modified HZSM-5.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"447 ","pages":"Article 116147"},"PeriodicalIF":6.5,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143842124","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}