Chinese Journal of Catalysis最新文献

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Efficient and selective photocatalytic CO2 conversion enabled by FePc nanosheets in a dye-sensitized system FePc纳米片在染料敏化系统中实现了高效和选择性的光催化CO2转化
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)65061-9
Hua Gao, Yong Zhu, Zhibing Wen, Ran Zhao, Zhi Chen, Siyao Wang, Shuanglin He, Kuang Peng, Yiwen Tang, Licheng Sun, Fei Li
{"title":"Efficient and selective photocatalytic CO2 conversion enabled by FePc nanosheets in a dye-sensitized system","authors":"Hua Gao,&nbsp;Yong Zhu,&nbsp;Zhibing Wen,&nbsp;Ran Zhao,&nbsp;Zhi Chen,&nbsp;Siyao Wang,&nbsp;Shuanglin He,&nbsp;Kuang Peng,&nbsp;Yiwen Tang,&nbsp;Licheng Sun,&nbsp;Fei Li","doi":"10.1016/S1872-2067(26)65061-9","DOIUrl":"10.1016/S1872-2067(26)65061-9","url":null,"abstract":"<div><div>Solar-driven photocatalytic CO<sub>2</sub> conversion offers a sustainable solution for greenhouse gas mitigation and renewable energy storage. While metal phthalocyanines (MPc) exhibit excellent CO<sub>2</sub> reduction capabilities, their practical application in dispersed photocatalytic systems faces limitations of the stacking of MPc molecules that reduces active site accessibility, and inefficient electron transfer limited by diffusive mass transport. To address these challenges, we developed a bioinspired dye-sensitized RuP-TiO<sub>2</sub>-FePc nanosheets (NSs) hybrid system, where ultrathin FePc NSs obtained by liquid-phase ultrasonic exfoliation enhance active site exposure and mass transfer, while TiO<sub>2</sub> serves as a mediator to facilitate electron transfer between the photosensitizer and FePc NSs. Time-resolved spectroscopic studies demonstrate that TiO<sub>2</sub> plays a dual role: it spatially organizes functional components to enable surface electron transfer by shortening intermolecular distances, while also functioning as a semiconductor bridge to facilitate charge transport. This synergistic design achieves a remarkable CO production rate of 27.3 mmol g<sup>–1</sup> h<sup>–1</sup> (&gt; 98% selectivity) and exceptional stability (TON<sub>CO</sub> = 1363 over 100 h), outperforming many noble-metal-based systems. Our work demonstrates a robust strategy for optimizing bulk catalysts through 2D exfoliation and controlled heterogenization, offering a versatile platform for efficient and durable artificial photosynthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 350-362"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558667","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
A van der Waals S-scheme homojunction in g-C3N4 g-C3N4中van der Waals S-scheme同结
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)65057-7
Ruchun Li, Liuyang Zhang
{"title":"A van der Waals S-scheme homojunction in g-C3N4","authors":"Ruchun Li,&nbsp;Liuyang Zhang","doi":"10.1016/S1872-2067(26)65057-7","DOIUrl":"10.1016/S1872-2067(26)65057-7","url":null,"abstract":"","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 1-4"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559105","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
Lanthanum-mediated single-atom dispersion of Ir and Dynamic oxygen replenishment in acidic water oxidation 镧介导的Ir单原子分散和酸性水氧化中的动态氧补充
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)65056-5
Chen Cao, Shirui Cui, Feng Shi, Yanqin Li, Chunyang Zhao, Wei Hu, Zelong Li, Yu Tang
{"title":"Lanthanum-mediated single-atom dispersion of Ir and Dynamic oxygen replenishment in acidic water oxidation","authors":"Chen Cao,&nbsp;Shirui Cui,&nbsp;Feng Shi,&nbsp;Yanqin Li,&nbsp;Chunyang Zhao,&nbsp;Wei Hu,&nbsp;Zelong Li,&nbsp;Yu Tang","doi":"10.1016/S1872-2067(26)65056-5","DOIUrl":"10.1016/S1872-2067(26)65056-5","url":null,"abstract":"<div><div>High-performance single-atom iridium (Ir) catalysts offer ultrahigh atomic utilization and can lower proton exchange membrane water electrolysis costs, but their improved oxygen evolution reaction (OER) activity often sacrifices stability. Here, incorporation of lanthanum (La) enables atomic dispersion of Ir on cobalt spinel (Co<sub>3</sub>O<sub>4</sub>) surface and shifts the Ir active-site OER pathway from the conventional adsorbate evolution mechanism to a lattice oxygen-mediated mechanism (LOM). The strongly oxophilic La sites tune the local electronic structure of Ir and accelerate interfacial water dissociation, enabling real-time replenishment of lattice oxygen consumed during LOM that a key process mitigates catalyst degradation. Consequently, Ir/CoLaO<sub><em>x</em></sub> shows an overpotential of 215 mV at 10 mA cm<sup>–2</sup> in acid and sustains 200 mA cm<sup>–2</sup> operation for 300 h in a full proton exchange membrane water electrolysis. This work provides a mechanistic framework for dynamic oxygen replenishment to stabilize lattice-oxygen catalysis and offers a strategy for designing atomically dispersed Ir catalysts for efficient, durable acidic OER.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 236-243"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558650","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
Synergistic optimization of interfacial electron transfer and surface hydrogen adsorption in a CdS/ZnO S-scheme heterojunction by site-specific doping: A DFT study 位点特异性掺杂对CdS/ZnO S-scheme异质结中界面电子转移和表面氢吸附的协同优化:DFT研究
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)65060-7
Yatai Zhou, Chengcheng Yuan, Wei Xia, Jun Wang, Xiaofeng Zhu, Yong Zhang, Bicheng Zhu, Jiaguo Yu
{"title":"Synergistic optimization of interfacial electron transfer and surface hydrogen adsorption in a CdS/ZnO S-scheme heterojunction by site-specific doping: A DFT study","authors":"Yatai Zhou,&nbsp;Chengcheng Yuan,&nbsp;Wei Xia,&nbsp;Jun Wang,&nbsp;Xiaofeng Zhu,&nbsp;Yong Zhang,&nbsp;Bicheng Zhu,&nbsp;Jiaguo Yu","doi":"10.1016/S1872-2067(26)65060-7","DOIUrl":"10.1016/S1872-2067(26)65060-7","url":null,"abstract":"<div><div>Fine-tuning the interfacial electronic interaction and surface reactivity of S-scheme heterojunctions is critical for advancing their photocatalytic performance. This study employs density functional theory calculations to systematically investigate the effects of transition metal (TM = Cr, Mn, Fe, Co, and Ni) doping at distinct sites of a CdS/ZnO S-scheme heterojunction: the surface (TM<sub>s</sub>), the interface (TM<sub>i</sub>), and co-doping at both sites (TM<sub>s+i</sub>). The results demonstrate that all doping configurations concurrently enhance both interfacial electron transfer and the hydrogen evolution reaction dynamics. The augmentation of electron transfer across the interface is primarily driven by TM doping at the interface, which reduces the work function of CdS and enlarges the Fermi level discrepancy with ZnO, leading to an enhancement trend of TM<sub>s+i</sub> &gt; TM<sub>i</sub> &gt; TM<sub>s</sub>. Conversely, the optimization of hydrogen adsorption free energy (Δ<em>G</em><sub>H*</sub>) is chiefly governed by surface TM doping, which downshifts the <em>p</em>-band center of S atoms and weakens the S–H bond, resulting in an improvement trend of TM<sub>s+i</sub> &gt; TM<sub>s</sub> &gt; TM<sub>i</sub>. Remarkably, the co-doping configuration exhibits a pronounced synergistic effect, outperforming any single-site doping in optimizing both properties. Furthermore, a clear periodic trend is identified: the promotional effect of TM doping, from Cr to Ni, progressively diminishes for both charge separation and surface reaction, which is linked to the increasing work function and S <em>p</em>-band center. This work highlights the significant potential of a multi-site doping strategy for the synergistic engineering of charge transfer and surface reactions in S-scheme heterojunctions, offering valuable theoretical insights for the precise design of high-efficiency photocatalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 327-337"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558658","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
Boosting co-thermal coupled in-situ reduction of morphology- engineered carbonate via preparing distinct crystalline phases 通过制备不同晶相促进共热耦合原位还原形貌工程碳酸盐
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)65039-5
Shaokang Yu, Meng Dong, Ming Xu, Yijia Lv, Zhiyang Peng, Weitao Zhang, Dabing Guo, Yixie Wang, Zhen Xue, Yusen Yang, Hao Li, Mingfei Shao
{"title":"Boosting co-thermal coupled in-situ reduction of morphology- engineered carbonate via preparing distinct crystalline phases","authors":"Shaokang Yu,&nbsp;Meng Dong,&nbsp;Ming Xu,&nbsp;Yijia Lv,&nbsp;Zhiyang Peng,&nbsp;Weitao Zhang,&nbsp;Dabing Guo,&nbsp;Yixie Wang,&nbsp;Zhen Xue,&nbsp;Yusen Yang,&nbsp;Hao Li,&nbsp;Mingfei Shao","doi":"10.1016/S1872-2067(26)65039-5","DOIUrl":"10.1016/S1872-2067(26)65039-5","url":null,"abstract":"<div><div>Co-thermal coupled <em>in-situ</em> hydrogenation of carbonates represents a promising strategy for producing metal oxide coupling syngas, facilitating the CO<sub>2</sub> conversion into value-added chemicals while reducing thermal decomposition temperatures. Nevertheless, the impact of CaCO<sub>3</sub> morphological modulation on hydrogenation performance and mechanisms has yet to be elucidated. Herein, we first report the morphology-controlled synthesis of CaCO<sub>3</sub> with distinct crystalline phases (<em>e.g.</em>, rhombohedral calcite, spherical vaterite, and rod-shaped aragonite). This engineered morphology significantly enhances co-thermal coupled in-situ reduction, simultaneously lowering the decarboxylation temperature and promoting syngas formation. Compared with rhombohedral calcite, spherical vaterite exhibits superior CO selectivity and formation rate during reduction processes across various temperatures, reaching 96% and 0.80 mmol min<sup>–1</sup> at 700 °C, respectively. Notably, rod-shaped aragonite achieves an exceptional CO selectivity of 86%, surpassing both rhombohedral calcite and spherical vaterite, and the CO formation rate (0.46 mmol min<sup>–1</sup>) is more than 2.3 times that of spherical vaterite at 550 °C. Moreover, combination of temperature programmed reduction-mass spectrometry and <em>in-situ</em> diffuse reflectance infrared Fourier transformed experiments reveals temperature-dependent hydrogenation mechanisms for different morphologies of CaCO<sub>3</sub>: direct hydrogenation dominates at relatively low temperatures, while at elevated temperatures, the dual mechanism combining direct hydrogenation and reverse water-gas shift reaction (HCOO* as the key intermediate) prevails. This study presents a novel strategy demonstrating high efficiency and low carbon for sustainable carbonate hydrogenation systems, offering significant scientific merit and industrial potential.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 149-159"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559091","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
Designing photocatalysts with selective oxygen reactivity for solar-driven methane coupling 设计具有选择性氧反应活性的太阳能驱动甲烷偶联光催化剂
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)65058-9
Shumin Zhang, Difa Xu, Wenjun Zhu
{"title":"Designing photocatalysts with selective oxygen reactivity for solar-driven methane coupling","authors":"Shumin Zhang,&nbsp;Difa Xu,&nbsp;Wenjun Zhu","doi":"10.1016/S1872-2067(26)65058-9","DOIUrl":"10.1016/S1872-2067(26)65058-9","url":null,"abstract":"","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 5-8"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559106","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
Chromium-driven lattice oxygen activation in high-entropy oxide for efficient oxygen evolution reaction 高熵氧化物中铬驱动晶格氧活化的高效析氧反应
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)65069-3
Qiurong Wang, Fozia Sultana, Renkun Li, Yan Fang, Selvi Mushina, Mingwu Tan, Tongtong Li, Renhong Li
{"title":"Chromium-driven lattice oxygen activation in high-entropy oxide for efficient oxygen evolution reaction","authors":"Qiurong Wang,&nbsp;Fozia Sultana,&nbsp;Renkun Li,&nbsp;Yan Fang,&nbsp;Selvi Mushina,&nbsp;Mingwu Tan,&nbsp;Tongtong Li,&nbsp;Renhong Li","doi":"10.1016/S1872-2067(26)65069-3","DOIUrl":"10.1016/S1872-2067(26)65069-3","url":null,"abstract":"<div><div>High-entropy oxides (HEOs) have emerged as promising electrocatalysts for the oxygen evolution reaction (OER) due to their unique tunable electronic structures and multi-site synergistic effects. Triggering the lattice oxygen oxidation mechanism (LOM) is considered an effective strategy to overcome the intrinsic limitations of the conventional adsorbate evolution mechanism (AEM). However, promoting the shift from AEM to LOM requires highly oxidized metal centers. Herein, we report on the rational design and synthesis of a (FeNiMoMnCr)<sub>3</sub>O<sub>4</sub>/NF HEO catalyst, wherein the introduction of high-valent Cr species serves as an electronic modulator to facilitate lattice-oxygen activity. The resulting catalyst exhibits a low overpotential of 248 mV at 100 mA cm<sup>–2</sup> in 1 mol L<sup>–1</sup> KOH and demonstrates excellent operational durability over 100 hours under high current densities. Comprehensive investigations, including pH-dependent electrochemical measurements, radical trapping experiments, and density functional theory calculations, reveal that the incorporation of Cr induces the in-situ formation of oxygen vacancies, thereby activating lattice-oxygen participation in the OER. This activation breaks the conventional linear scaling relationships associated with AEM, leading to enhanced reaction kinetics. This study provides mechanistic insights into how high-valent metals regulate electronic structure and lattice oxygen reactivity in HEOs, offering a feasible design strategy for advanced OER electrocatalysts based on the LOM pathway.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 277-289"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558654","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
WO2.72-modulated Ru cluster boosting dual-site adsorption for efficient and CO-resistant anion exchange membrane fuel cells wo2.72调制Ru簇促进高效耐co阴离子交换膜燃料电池的双点吸附
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)65066-8
Xu Yu, Han Tian, Ziyi Yu, Fantao Kong, Min Wang, Ruxiang Shen, Xiangzhi Cui, Jianlin Shi
{"title":"WO2.72-modulated Ru cluster boosting dual-site adsorption for efficient and CO-resistant anion exchange membrane fuel cells","authors":"Xu Yu,&nbsp;Han Tian,&nbsp;Ziyi Yu,&nbsp;Fantao Kong,&nbsp;Min Wang,&nbsp;Ruxiang Shen,&nbsp;Xiangzhi Cui,&nbsp;Jianlin Shi","doi":"10.1016/S1872-2067(26)65066-8","DOIUrl":"10.1016/S1872-2067(26)65066-8","url":null,"abstract":"<div><div>A dual-site synergistic catalytic mechanism is proposed to optimize the OHad binding energy (OHBE) by constructing ultrafine Ru nanoclusters modified with highly oxygenophilic WO<sub>2.72</sub> clusters in nitrogen-doped carbon carriers, which can optimize the adsorptions of OH<sub>ad</sub> and active hydrogen species, respectively, resulting in a marked increase in hydrogen oxidation reaction (HOR) activity. The constructed Ru-WO<sub>2.72</sub>-NC shows a HOR mass activity about 8 times that of Pt-C, and the corresponding alkaline exchange membrane fuel cells demonstrate rather higher peak power densities than Ru-NC with 1.193 W cm<sup>–2</sup> and more than 1 W cm<sup>–2</sup> in H₂ fuel and CO/H<sub>2</sub> mixtures, respectively. The excellent alkaline HOR performance of Ru-WO<sub>2.72</sub>-NC is attributed to the adsorption of OH<sub>ad</sub> species by WO<sub>2.72</sub> clusters, which synergizes with the adsorption and dissociation of hydrogen on Ru to facilitate the Volmer step. The success in constructing dual-site synergistic catalysis of Ru-WO<sub>2.72</sub>-NC anode provides valuable insight and new guidelines for designing and studying high-activity alkaline HOR catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 302-314"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558656","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
Silica-confined Cu2O nanoparticles for propylene epoxidation with molecular oxygen 二氧化硅纳米Cu2O用于丙烯与分子氧的环氧化
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)65059-0
Jiawei Cheng, Kai Wang, Yuhan Meng, Jiachen Wang, Zuozheng Liu, Jingjuan Wang, Jiaxu Liu, Kang Cheng, Qinghong Zhang, Ye Wang
{"title":"Silica-confined Cu2O nanoparticles for propylene epoxidation with molecular oxygen","authors":"Jiawei Cheng,&nbsp;Kai Wang,&nbsp;Yuhan Meng,&nbsp;Jiachen Wang,&nbsp;Zuozheng Liu,&nbsp;Jingjuan Wang,&nbsp;Jiaxu Liu,&nbsp;Kang Cheng,&nbsp;Qinghong Zhang,&nbsp;Ye Wang","doi":"10.1016/S1872-2067(26)65059-0","DOIUrl":"10.1016/S1872-2067(26)65059-0","url":null,"abstract":"<div><div>The direct propylene epoxidation with molecular oxygen offers an atom-economical route to propylene oxide (PO). However, the oxidative reaction conditions required at high temperatures often induce complete propylene oxidation and the reconstruction of the active centers, compromising PO selectivity. Herein, we propose a redispersion-confinement strategy to encapsulate small, low-valence Cu nanoparticles (NPs) within a silica shell, thereby achieving stable dispersion across various supports. We confirm that the formation of Cu-O-Si coordination between Cu and silica, together with cesium promotion, could stabilize the small Cu NPs and enhance the PO formation. The optimum Cs-Cu@Si/SBA-15 catalyst delivers a 3.9% propylene conversion and a 68% PO selectivity, markedly surpassing the 0.6% conversion and 42% selectivity obtained over Cs-Cu/SBA-15 without the silica shell. A significant space and chemical state confinement effect is evidenced between CuO and the silica shell, which retards the reactivity of lattice oxygen and allows the moderate activation of molecular oxygen to electrophilic oxygen species; thus, promoting the selective epoxidation of propylene. This strategy offers a general approach for molecular-level control of active-site structure and electronic states in heterogeneous catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 77-88"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148559085","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
Ligand-defect synergistic catalyst for localized CO2 concentration enhancement in electrochemical reduction of low concentration CO2 配体缺陷协同催化剂在低浓度CO2电化学还原中局部增强CO2浓度
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)65031-0
Junyan Liu, Tao Shao, Xun Peng, Shengwei Liu
{"title":"Ligand-defect synergistic catalyst for localized CO2 concentration enhancement in electrochemical reduction of low concentration CO2","authors":"Junyan Liu,&nbsp;Tao Shao,&nbsp;Xun Peng,&nbsp;Shengwei Liu","doi":"10.1016/S1872-2067(26)65031-0","DOIUrl":"10.1016/S1872-2067(26)65031-0","url":null,"abstract":"<div><div>Electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) is a potential strategy for mitigating severe greenhouse effect. Despite its potential, CO<sub>2</sub>RR encounters critical challenges to convert low CO<sub>2</sub> concentrations in practical scenarios, due to the CO<sub>2</sub> mass transfer limitations. Herein, we prepared a reduced 2-aminoterephthalic acid modified bismuth coordination compound (Re-BiBDC-NH<sub>2</sub>) for CO<sub>2</sub>RR in low CO<sub>2</sub> concentrations. Retained amino groups after in situ reduction induce abundant unsaturated coordination sites, enhancing CO<sub>2</sub> adsorption and enabling localized concentration enhancement even under low CO<sub>2</sub> supply concentrations. As such, the optimized Re-BiBDC-NH<sub>2</sub> achieves a Faradaic efficiency for formate (FE<sub>formate</sub>) of &gt; 80% at a wide potential range of 700 mV, FE<sub>formate</sub> of &gt;75% across 15%–100% CO<sub>2</sub> concentrations. Furthermore, in a flow cell at a current density of 300 mA cm⁻<sup>2</sup> and across a wide pH range (pH = 1.7, 7, and 14), the Re-BiBDC-NH<sub>2</sub> catalyst achieved FE<sub>formate</sub> &gt; 95%, with a single-pass carbon efficiency (SPCE) reaching 71.6% in acidic electrolyte (pH = 1.7). In situ spectroscopies and Density functional theory calculations reveal that dynamically frustrated Lewis pairs formed by amino groups and defects concentrate CO<sub>2</sub>, and stabilize *OCHO intermediates to reduce energy barriers, thereby not only enhancing the CO<sub>2</sub>RR performance but also allowing reaction to operate under low CO<sub>2</sub> concentrations. This work presents a promising ligand-defect synergistic catalyst for low-concentration CO<sub>2</sub>RR, offering insights for bridging catalyst research and practical CO<sub>2</sub> conversion.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"86 ","pages":"Pages 265-276"},"PeriodicalIF":17.2,"publicationDate":"2026-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148558653","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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