Chinese Journal of Catalysis最新文献

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Solvent-free chemical recycling of polyolefins and polystyrene under mild conditions via GaCl3-based molten catalysts 基于gacl3的熔融催化剂在温和条件下对聚烯烃和聚苯乙烯进行无溶剂化学回收
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65067-X
Lei Yuan, Zhiwen Gao, Libin Shi, Cuishi Guan, Dongyue Peng, Shuhui Fang, Wei Zhang, Yue Liu
{"title":"Solvent-free chemical recycling of polyolefins and polystyrene under mild conditions via GaCl3-based molten catalysts","authors":"Lei Yuan,&nbsp;Zhiwen Gao,&nbsp;Libin Shi,&nbsp;Cuishi Guan,&nbsp;Dongyue Peng,&nbsp;Shuhui Fang,&nbsp;Wei Zhang,&nbsp;Yue Liu","doi":"10.1016/S1872-2067(26)65067-X","DOIUrl":"10.1016/S1872-2067(26)65067-X","url":null,"abstract":"<div><div>The chemical recycling of polyolefins (PE, PP) and polystyrene (PS) remains a major challenge due to their chemical stability of C–C backbones as well as the limited accessibility of polymer chains to catalytic active sites. Here, we report a solvent-free, low-temperature, and synergistic depolymerization strategy using a GaCl<sub>3</sub>-based molten Lewis acid catalyst for the efficient conversion of PE, PP, and PS, both individually and in mixed plastics streams. The low melting point of the catalyst ensures liquid-phase mobility and efficient contact between polymer and catalysts, achieving complete PS conversion and over 60% PE/PP conversion within 30 min. In mixed plastics, a synergistic reaction pathway mediated by carbocation-type intermediates enables Friedel-Crafts alkylation between PS-derived aromatics and polyolefin-derived olefins, enhancing overall conversion (~85%) and selectivity toward mono-alkylated aromatics (up to 33.5%). Raman spectra confirmed the formation of [GaCl<sub>4</sub>]<sup>–</sup> and [Ga<sub>2</sub>Cl<sub>7</sub>]<sup>–</sup> chlorogallate species during the reaction. This study demonstrates a novel, integrated approach for solvent-free, selective, and energy-efficient chemical recycling of mixed plastics, highlighting GaCl<sub>3</sub>-based molten salts as versatile catalysts for circular and sustainable plastic recycling.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 137-148"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559090","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
Self-photosensitizing metal complexes for photocatalytic hydrogen evolution 用于光催化析氢的自光敏金属配合物
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65050-4
Mingyu Ma, Zongyang Liu, Kuo Yuan, Zheyuan Liu, Jiaxin Wang, Qingqing Lin, Di-Chang Zhong, Tong-Bu Lu
{"title":"Self-photosensitizing metal complexes for photocatalytic hydrogen evolution","authors":"Mingyu Ma,&nbsp;Zongyang Liu,&nbsp;Kuo Yuan,&nbsp;Zheyuan Liu,&nbsp;Jiaxin Wang,&nbsp;Qingqing Lin,&nbsp;Di-Chang Zhong,&nbsp;Tong-Bu Lu","doi":"10.1016/S1872-2067(26)65050-4","DOIUrl":"10.1016/S1872-2067(26)65050-4","url":null,"abstract":"<div><div>Combining organic photosensitive center with dinuclear-metal catalytic center through covalent bonds to synthesize supramolecular catalysts for photocatalytic hydrogen evolution is a cost-efficient approach to convert solar to hydrogen energy, while it has been rarely explored. Herein, we constructed a self-photosensitizing pyrene-decorated dinuclear cobalt(II) molecular photocatalyst [Co<sub>2</sub>(pyrene-L)<sub>2</sub>] <em>via</em> covalent bonds, which can accelerate photogenerated electron transfer from pyrene center to dinuclear cobalt(II) center, achieving efficiently photocatalytic hydrogen evolution in the absence of any noble metal photosensitizers. The photocatalytic activity of Co<sub>2</sub>(pyrene-L)<sub>2</sub> is more than 3-fold over that of the physically mixed sample. Moreover, owing to the synergistic effect of dinuclear cobalt(II) centers, the activity of Co<sub>2</sub>(pyrene-L)<sub>2</sub> is 10-fold higher than that of mononuclear counterpart (Co(pyrene-L)<sub>2</sub>). As the first example of self-photosensitizing pyrene-decorated dinuclear metal molecular catalyst, it not only features multi-functions of photosensitivity, photoreduction and photooxidation, but also possesses synergistic dinuclear metal centers to improve catalytic activity, which gives new insights for researchers in designing high-performance photocatalysts for hydrogen evolution.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 375-383"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558605","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
Atomic Bi substitution stabilized AgBi single-atom alloy with 4H/fcc heterophase interfaces for efficient CO2 reduction 具有4H/fcc异相界面的原子Bi取代稳定AgBi单原子合金,可有效还原CO2
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65090-5
Wenbo Wang, Shanhe Gong, Erjun Kan, Guoxing Zhu, Pengwei Huo, Jintong Guan, Xiaomeng Lv
{"title":"Atomic Bi substitution stabilized AgBi single-atom alloy with 4H/fcc heterophase interfaces for efficient CO2 reduction","authors":"Wenbo Wang,&nbsp;Shanhe Gong,&nbsp;Erjun Kan,&nbsp;Guoxing Zhu,&nbsp;Pengwei Huo,&nbsp;Jintong Guan,&nbsp;Xiaomeng Lv","doi":"10.1016/S1872-2067(26)65090-5","DOIUrl":"10.1016/S1872-2067(26)65090-5","url":null,"abstract":"<div><div>The pressing need to address global energy demand and climate change has positioned electrochemical CO<sub>2</sub> reduction into high-value chemicals as a crucial technology for carbon cycling and sustainable energy storage. However, precise control over the interfacial structure of active sites in single-atom alloy (SAA) remains a considerable challenge, significantly restricting their catalytic performance. In this study, we propose an atomic-level substitution strategy, integrating large atomic radius of Bi atoms into the Ag lattice to trigger and stabilize a 4H/fcc-Ag heterophase interfaces. Theoretical and experimental analyses reveal that the induced lattice strain stabilizes the metastable 4H phase and optimizes the geometric/electronic configuration of active sites, thereby enhancing the orbital overlap between Ag-3<em>d</em> and C-2<em>p</em> orbitals and lowering the energy barrier for *COOH formation. The optimal 4H/fcc Ag<sub>49</sub>Bi<sub>1</sub> SAA catalyst, comprising approximately 3% 4H-Ag and 97% fcc-Ag, achieves CO Faraday efficiency (FE<sub>CO</sub>) of 99.5%, single-pass conversion efficiency of 70%, CO yield of 45.6 mmol h<sup>−1</sup> cm<sup>−2</sup> and superior durability over 330 h under 200 mA cm<sup>−2</sup> in an alkaline flow cell. A membrane electrode assembly electrolyzer incorporating the catalyst reached a peak FE<sub>CO</sub> of 98.6% at 150 mA cm<sup>−2</sup> and maintaining FE<sub>CO</sub> &gt;80% for 70 h under 100 mA cm<sup>−2</sup> without decay. When applied in a customized Zn-CO<sub>2</sub> battery, it delivered a peak power density of 0.86 mW cm<sup>−2</sup>, along with 140 h cycling stability at 2 mA cm<sup>−2</sup>. This work underscores the potential of atomic-level substitution for precise interface engineering, providing a novel strain-engineering strategy for designing high-performance SAA catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 212-224"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558666","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
Interfacial two-site synergy for biomass electro-oxidation in a near-neutral electrolyte 近中性电解液中生物质电氧化界面的双向协同作用
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65041-3
Chenyu Bu, Zhuoran Lu, Zhongcheng Xia, Yun Fan, Cairong Wang, Yutong Huang, Shuangyin Wang, Yuqin Zou
{"title":"Interfacial two-site synergy for biomass electro-oxidation in a near-neutral electrolyte","authors":"Chenyu Bu,&nbsp;Zhuoran Lu,&nbsp;Zhongcheng Xia,&nbsp;Yun Fan,&nbsp;Cairong Wang,&nbsp;Yutong Huang,&nbsp;Shuangyin Wang,&nbsp;Yuqin Zou","doi":"10.1016/S1872-2067(26)65041-3","DOIUrl":"10.1016/S1872-2067(26)65041-3","url":null,"abstract":"<div><div>Electrocatalytic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) in a near-neutral electrolyte mitigates HMF polymerization, thereby enhancing catalyst stability for long-term operation. However, the insufficient supply of active oxygen species during the electro-oxidation process often leads to the formation of partially oxidized intermediates instead of the desired product, 2,5-furandicarboxylic acid (FDCA). In this study, an atomically dispersed ruthenium-loaded copper oxide electrocatalyst (Ru/CuO) is prepared to promote the generation of hydroxide (OH<sup>–</sup>) ions and facilitate complete HMF oxidation to FDCA. <em>In-situ</em> attenuated total reflectance surface-enhanced infrared absorption spectroscopy, density functional theory calculations, and quartz crystal microbalance mass analysis revealed that CuO serves as the active site for the HMF oxidation reaction (HMFOR), whereas the introduction of Ru single atoms accelerates OH<sup>–</sup> formation, lowers the reaction barrier for the key dehydrogenation steps in HMFOR, and enhances HMF adsorption. These features enable the Ru/CuO catalyst to deliver significantly improved low-potential oxidation performance under near-neutral conditions, reaching a 93% FDCA yield and 87.7% Faradaic efficiency at 1.15 V<sub>RHE</sub>, along with stable operation in a flow cell. This work demonstrates efficient conversion of HMF to FDCA in a near-neutral electrolyte and proposes a rational design strategy for HMFOR catalyst operating under near-neutral conditions.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 160-170"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148573818","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
Engineering channel microenvironment and charge dynamics in covalent organic frameworks through linkage-specific povarov cyclization for enhanced photocatalytic hydrogen evolution 工程通道微环境和电荷动力学在共价有机框架通过连接特异性波瓦洛夫环增强光催化氢演化
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65053-X
Hanxi Li, Zhendong Luo, Qiang Xue, Yunfei Zhi, Jun Du, Xukai Zhou
{"title":"Engineering channel microenvironment and charge dynamics in covalent organic frameworks through linkage-specific povarov cyclization for enhanced photocatalytic hydrogen evolution","authors":"Hanxi Li,&nbsp;Zhendong Luo,&nbsp;Qiang Xue,&nbsp;Yunfei Zhi,&nbsp;Jun Du,&nbsp;Xukai Zhou","doi":"10.1016/S1872-2067(26)65053-X","DOIUrl":"10.1016/S1872-2067(26)65053-X","url":null,"abstract":"<div><div>Covalent organic frameworks (COFs) offer a modular platform for photocatalytic hydrogen evolution (PHE), where linkage topology and channel architecture dictate charge separation and mass transport. However, the role of linkage isomerism in coupling pore microenvironments with photocatalytic function remains unclear. We synthesized COF-PQ and COF-DPPQ via in-situ Povarov cyclization of pyrene-based imine direction distinct intermediates, creating frameworks with identical building blocks but distinct donor-acceptor arrangements and pore microenvironments that underpin their contrasting catalytic behaviors. This structural divergence drives profound functional differences: COF-DPPQ achieves a PHE rate of 37.82 mmol g<sup>–1</sup> h<sup>–1</sup>, nearly 100-fold higher than COF-PQ. Mechanistically, COF-DPPQ exhibits lower electron effective mass (0.574 <em>vs</em>. 1.046), stronger donor-acceptor polarization (~0.95 |e| <em>vs</em>. ~0.24 |e|), prolonged carrier lifetimes (37.28 <em>vs</em>. 1.26 ps), and superior proton adsorption and diffusion (2.2-fold capacity; 0.916 × 10<sup>–3</sup> <em>vs</em>. 0.660 × 10<sup>–3</sup> cm<sup>2</sup> s<sup>–1</sup>). These results identify linkage topology as an effective lever to regulate exciton dynamics and mass transport, guiding the design of next-generation COF photocatalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 363-374"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558668","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
Recent advances in noble metal-based catalysts for methane decomposition: Performance, mechanism, and optimization 贵金属基甲烷分解催化剂的研究进展:性能、机理及优化
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65068-1
Shahla Karimi, Mehran Rezaei, Jiguang Deng, Hongxing Dai, Ali Rastegarpanah
{"title":"Recent advances in noble metal-based catalysts for methane decomposition: Performance, mechanism, and optimization","authors":"Shahla Karimi,&nbsp;Mehran Rezaei,&nbsp;Jiguang Deng,&nbsp;Hongxing Dai,&nbsp;Ali Rastegarpanah","doi":"10.1016/S1872-2067(26)65068-1","DOIUrl":"10.1016/S1872-2067(26)65068-1","url":null,"abstract":"<div><div>Excessive greenhouse gas emissions from fossil fuel consumption, particularly in energy-dependent sectors, highlight the urgent need for cleaner alternatives such as hydrogen as a promising energy source. Methane decomposition (MD) is a key milestone in the production of CO<sub><em>x</em></sub>-free fuels, while producing valuable carbon nanomaterials, and commonly used catalysts include metallic oxides and noble metals. Noble metals have attracted wide attention because of their unique electronic structures and good catalytic qualities. Hence, initially, this review systematically focuses on the performance of noble metal catalysts, including Pt, Pd, Rh, Ru, Ir, and Au in the methane decomposition process, highlighting their distinct reaction mechanisms and active site behaviors. Beyond serving as active catalytic components, special attention is placed on the promotional behavior of noble metals, which, when incorporated with transition metals, can tune electronic interactions, increase dispersion, and suppress deactivation, offering a new perspective on their dual functionality in methane decomposition catalysis. Additionally, the influence of reaction conditions, including WHSV, feed ratio, and CH<sub>4</sub> partial pressure, is examined to correlate reaction conditions with catalytic performance. The next objective also encompasses strategies for improving catalytic performance, such as evaluating various active sites, exploring synthesis strategies, investigating the nature of the supports, examining the presence of promoters, and utilizing plasma-assisted reduction. The final section of this review provides a roadmap for future development of high-performance, cost-effective, and durable noble metal-based catalysts for efficient methane decomposition.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 9-48"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559083","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
Fe-based catalyst for thermo-catalytic CO2 hydrogenation into ethanol: The essential role of water management and Fe-based carbide/oxide ratio 热催化CO2加氢制乙醇的铁基催化剂:水管理和铁基碳化物/氧化物比的重要作用
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65065-6
Xiaojie Liu, Zhifu Yu, Qi Li, Yang Wang, Xinze Bi, Kaixuan Huo, Dingyao Li, Zhiang Yuan, Yifan Yan, Shibin Li, Yiwu Lu, Qiang Liu, Wenhang Wang, Mingbo Wu
{"title":"Fe-based catalyst for thermo-catalytic CO2 hydrogenation into ethanol: The essential role of water management and Fe-based carbide/oxide ratio","authors":"Xiaojie Liu,&nbsp;Zhifu Yu,&nbsp;Qi Li,&nbsp;Yang Wang,&nbsp;Xinze Bi,&nbsp;Kaixuan Huo,&nbsp;Dingyao Li,&nbsp;Zhiang Yuan,&nbsp;Yifan Yan,&nbsp;Shibin Li,&nbsp;Yiwu Lu,&nbsp;Qiang Liu,&nbsp;Wenhang Wang,&nbsp;Mingbo Wu","doi":"10.1016/S1872-2067(26)65065-6","DOIUrl":"10.1016/S1872-2067(26)65065-6","url":null,"abstract":"<div><div>CO<sub>2</sub> hydrogenation to ethanol represents a pivotal pathway for valuable utilization of greenhouse gas CO<sub>2</sub>, yet conventional catalysts are still limited by active-phase instability and undesirable byproduct selectivity. Herein, we propose a dual-components catalyst system synergized by hydrophobic carbon-encapsulated Fe-based catalyst (NaFe@C) and K modified CuZnAl component (KCZA), which achieves ultra-high ethanol selectivity of 35% under optimized conditions (5 MPa and 320 °C). KCZA initiates the CO<sub>2</sub> activation <em>via</em> reverse water-gas shift reaction and supplies oxygen-containing intermediates (mainly CH<sub><em>x</em></sub>O*, <em>x</em> = 0, 1, or 2). NaFe@C component is mainly responsible for the C–O activation for CH<sub><em>x</em></sub>* formation and C–C coupling between CH<sub><em>x</em></sub>* and CH<sub><em>x</em></sub>O*, as well as the following hydrogenation step for ethanol synthesis. Notably, the hydrophobic carbon shell in NaFe@C plays a critical role in tailoring the oxidation behaviors of Fe-based active sites and optimizing the phase ratio of Fe<sub>3</sub>O<sub>4</sub>/<em>χ</em>-Fe<sub>5</sub>C<sub>2</sub> via water management. Multiple characterization and theoretical simulation results clarify that the unique electronic property of Fe-based active sites endowed by the optimized phase ratio is beneficial to boost the ethanol synthesis performance by balancing the coverage of key intermediates and lowering the energy barrier of essential steps. This work is promising to provide guidance for the rational design of advanced catalysts for targeted transformation of CO<sub>2</sub> or syngas into ethanol and beyond.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 112-124"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559088","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
Decoupling competitive reactions by their differential orbital-coupling response to vacancy engineering for efficient electrocatalytic nitrogen reduction 竞争反应的微分轨道耦合解耦与空位工程的高效电催化氮还原
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65043-7
Dezhi Wang, Songhua Yang, Yiyi Yangliu, Xufa Peng, Fangyang Liu, Hao Fei, Zhuangzhi Wu
{"title":"Decoupling competitive reactions by their differential orbital-coupling response to vacancy engineering for efficient electrocatalytic nitrogen reduction","authors":"Dezhi Wang,&nbsp;Songhua Yang,&nbsp;Yiyi Yangliu,&nbsp;Xufa Peng,&nbsp;Fangyang Liu,&nbsp;Hao Fei,&nbsp;Zhuangzhi Wu","doi":"10.1016/S1872-2067(26)65043-7","DOIUrl":"10.1016/S1872-2067(26)65043-7","url":null,"abstract":"<div><div>The electrocatalytic nitrogen reduction reaction (NRR) poses formidable challenges, such as competing hydrogen evolution and poor N<sub>2</sub> activation. Herein, we introduce a precise electronic-structure tuning modality through controlled sulfur vacancy (V<sub>S</sub>) engineering in 1T-MoS<sub>2</sub>. By manipulating the V<sub>S</sub> concentration to nearly 9.38%, the optimized catalyst (MoS<sub>2</sub>-100) achieves an outstanding NH<sub>3</sub> yield of 64.50 μg h<sup>–1</sup> mg<sup>–1</sup> and a Faradaic efficiency of 15.25%, superior to most electrocatalysts reported. Mechanistic studies reveal that enhanced <em>d</em>-<em>σ</em> orbital coupling between Mo and N<sub>2</sub> significantly promotes N<sub>2</sub> activation, while the distinct orbital-coupling responses of Mo–N<sub>2</sub> and Mo–H to V<sub>S</sub> concentration render a potential competition-preponderance window for NRR. This work establishes a novel paradigm for decoupling the competitive reactions by utilizing their differential sensitivity of orbital coupling to vacancy engineering.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 181-190"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559093","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
The C–C bond cleavage inhibition and intermediates adsorption enhancement co-boost the selective electrooxidation of ethylene glycol on silver-palladium hollow nanocubes C-C键解理抑制和中间体吸附增强共同促进了乙二醇在银钯空心纳米立方上的选择性电氧化
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65015-2
Zi-Hang Wang, Wei Zhong, Si-Qi Li, Bin Sun, Hao Lan, Xiao-Yu Zhang, Xin Wang, Yu Chen, Xuan Ai
{"title":"The C–C bond cleavage inhibition and intermediates adsorption enhancement co-boost the selective electrooxidation of ethylene glycol on silver-palladium hollow nanocubes","authors":"Zi-Hang Wang,&nbsp;Wei Zhong,&nbsp;Si-Qi Li,&nbsp;Bin Sun,&nbsp;Hao Lan,&nbsp;Xiao-Yu Zhang,&nbsp;Xin Wang,&nbsp;Yu Chen,&nbsp;Xuan Ai","doi":"10.1016/S1872-2067(26)65015-2","DOIUrl":"10.1016/S1872-2067(26)65015-2","url":null,"abstract":"<div><div>Efficient electrooxidation of ethylene glycol (EG) to glycolic acid (GA) is highly desirable for biomass valorization and EG recycling, which remains challenging owing to side reactions involving C–C bond cleavage. Herein, the bimetallic AgPd hollow nanocubes (AgPd hNCs) are successfully prepared via a solvothermal-assisted Galvanic replacement strategy. Both theoretical calculations and experimental results indicate that the electronic interplay between the Pd atom and Ag atom hinders C–C bond breaking and enhances the adsorption of critical intermediates, resulting in high selectivity toward GA production. Benefiting from these features, AgPd hNCs achieve a Faradaic efficiency of 93% toward GA formation and a 2.8-fold increase in mass activity compared to Pd black. Moreover, the strong oxygen affinity of Ag promotes the removal of CO-like intermediates from the Pd surface, resulting in superior EG oxidation stability. This study highlights a generalizable Ag-based strategy to modulate bimetallic interfaces for selective oxidation reaction of specific functional groups, contributing to the rational design of electrocatalysts for biomass upgrading.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 191-200"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559094","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
Interfacial charge manipulation enhancing H-bond connectivity for promoted oxygen evolution 界面电荷操纵增强氢键连通性以促进氧的析出
IF 17.2 1区 化学
Chinese Journal of Catalysis Pub Date : 2026-07-01 Epub Date: 2026-07-02 DOI: 10.1016/S1872-2067(26)65070-X
Jun Ke, Jiaxi Zhang, Longhai Zhang, Chengzhi Zhong, Huiyu Song, Li Du, Yuwei Zhang, Zhiming Cui
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