Chinese Journal of Catalysis最新文献

Light-switchable product selectivity in CO2 photoreduction over hollow plasmonic TiO2/AuCu@COF core-shell architectures 空心等离子体TiO2/AuCu@COF核壳结构中CO2光还原的光开关产物选择性

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65075-9

Xin Yuan, Linyi Wu, Fengying Cao, Lechu Xu, Peng Wang, Hulin Shi, Shuxian Zhong, Lian Liu, Weihao Mo, Leihong Zhao, Song Bai

{"title":"Light-switchable product selectivity in CO2 photoreduction over hollow plasmonic TiO2/AuCu@COF core-shell architectures","authors":"Xin Yuan, Linyi Wu, Fengying Cao, Lechu Xu, Peng Wang, Hulin Shi, Shuxian Zhong, Lian Liu, Weihao Mo, Leihong Zhao, Song Bai","doi":"10.1016/S1872-2067(26)65075-9","DOIUrl":"10.1016/S1872-2067(26)65075-9","url":null,"abstract":"<div><div>The development of photo-switchable CO2 reduction catalysts capable of selectively generating two distinct target products under different light irradiation holds significant potential for achieving multifunctional catalysis and enhancing economic viability in industrial applications, yet remains a formidable challenge. Herein, we demonstrate a hollow core-shell plasmonic TiO2/AuCu@TB-COF (TACT) photocatalyst that achieves 343.9 μmol gcat–1 h–1 activity and 98.7% selectivity toward CH4 under ultraviolet (UV) light, but switches to 132.7 μmol gcat–1 h–1 activity with 86.6% selectivity for CO under visible light in pure water without altering any other reaction conditions. Comprehensive mechanistic studies reveal that UV and visible light selectively excite different components, inducing distinct interfacial charge transfer routes. This not only endows TACT with higher charge separation efficiency under UV light versus visible light, but also directs photocarriers to different active sites for redox reactions depending on the irradiation wavelength. Specifically, H2O oxidation occurring on the TiO2 core under UV light more favorably promotes O2 evolution and proton liberation compared to oxidation on the TB-COF shell under visible light. For CO2 reduction, UV light drives consecutive hydrogenation of *CO intermediates on the AuCu sites, whereas visible light preferentially induces *CO desorption from the TB-COF surface. The contrasting electron and proton supply, combined with the divergent fates of *CO intermediates, collectively govern the wavelength-dependent CO2 reduction pathways.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 87-99"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651898","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

Electrosynthesis of nylon-6 precursor via heteroatom-doping- regulated oxygen vacancies engineering over ZnO ZnO上杂原子掺杂调控氧空位工程电合成尼龙-6前驱体

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65062-0

Suwei Lu, Hongping Yan, Hongwei Zhang, Yuying Cheng, Xinxin Jiang, Xuyun Peng, Junwei Huang, Yuanjin Li, Xin Wang, Shijing Liang, Lilong Jiang

{"title":"Electrosynthesis of nylon-6 precursor via heteroatom-doping- regulated oxygen vacancies engineering over ZnO","authors":"Suwei Lu, Hongping Yan, Hongwei Zhang, Yuying Cheng, Xinxin Jiang, Xuyun Peng, Junwei Huang, Yuanjin Li, Xin Wang, Shijing Liang, Lilong Jiang","doi":"10.1016/S1872-2067(26)65062-0","DOIUrl":"10.1016/S1872-2067(26)65062-0","url":null,"abstract":"<div><div>Electrocatalysis is a green alternative to directly synthesize cyclohexanone oxime (CHOX, Nylon-6 precursor) via electrocatalytic reduction of nitrogen oxides to NH2OH and spontaneous C–N coupling with cyclohexanone, but suffering from a low-yield or poor Faradaic efficiency (FE) because of the scaling relationship. Herein, a strategy of heteroatom-doping-regulated oxygen vacancies (Vo) engineering was proposed to design a robust Cu-ZnO1−x catalyst for efficient electrosynthesis of cyclohexanone oxime (ESCO). The complete characterizations and theoretical studies revealed that the doped-Cu can reduce Vo sites formation energy and regulate their local electronic state. The synergistic effect between doped Cu and Vo led to the break of the scaling relationship, presenting the enhancement of NO3− adsorption/dissociation, the weakness of H* adsorption, and the balance of the NH2OH adsorption for further C–N coupling reaction. Therefore, the hydrogen evolution reaction and NH2OH reduction to NH3 side reactions can be suppressed. The optimized Cu-ZnO1−x delivered an outstanding activity with a 1238.8 μmol h−1 mgcat.−1 yield and 68.2% FE. Lastly, the reaction mechanism was established following *NO3 → *NO3H → *NO2 → *NO2H → *NO → *HNO → *NHOH → *NH2OH and spontaneous C–N coupling with cyclohexanone to form CHOX. The outstanding ESCO performance on Cu-ZnO1−x catalyst demonstrates the effectiveness of this heteroatom-doping-regulated Vo engineering strategy.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 243-253"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651904","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

Unveiling the dominant distal-alternating hybrid mechanism in B-modulated Mo2TiC2Tx/MoO2 MXene for highly selective ambient NRR 揭示了b调制Mo2TiC2Tx/MoO2 MXene在高选择性环境NRR中的主要远端交替混合机制

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65080-2

Fengjuan Guo, Chunyao Ma, Yue Huang, Sitong Hang, Junwei Ma, Hongtao Gao

{"title":"Unveiling the dominant distal-alternating hybrid mechanism in B-modulated Mo2TiC2Tx/MoO2 MXene for highly selective ambient NRR","authors":"Fengjuan Guo, Chunyao Ma, Yue Huang, Sitong Hang, Junwei Ma, Hongtao Gao","doi":"10.1016/S1872-2067(26)65080-2","DOIUrl":"10.1016/S1872-2067(26)65080-2","url":null,"abstract":"<div><div>Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions offers a sustainable alternative to the energy-intensive Haber-Bosch process. However, the two canonical catalytic pathways face intrinsic limitations: the alternating mechanism suffers from high *NH2NH2 desorption losses, while the distal pathway requires prohibitive activation energy for N2 protonation. The simultaneous realization of high activity and selectivity thus remains a critical challenge. Here, we demonstrate that boron doping modulates the electronic structure of Mo2TiC2Tx/MoO2 by upshifting the d-/p-band center toward the Fermi level, unveiling the dominant a hybrid “distal-alternating” pathway that favors the *NNHH → *NHNH2 transition rather than the *NNHH → *N cleavage. In addition, the electron-deficient B sites weaken the binding affinity toward Lewis-acidic protons under acidic conditions, thereby effectively suppressing the competing hydrogen evolution reaction. Significant interfacial charge transfer from MoO2 to the B@Mo2TiC2Tx surface further ensures a sufficient electron supply for N2 activation and stepwise hydrogenation. As a result, B@Mo2TiC2Tx/MoO2 delivers an impressive ammonia yield of 121.18 μg h−1 mgcat.−1 with a Faradaic efficiency of 75.94% at a mild potential of –0.2 V vs. RHE. This work unveils the mechanistic feasibility of a non-classical hybrid NRR pathway and establishes a rational strategy for designing next-generation high-efficiency nitrogen reduction electrocatalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 269-281"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651907","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 chloride resistance via hydrogen−bond network dynamic optimization and electrostatic repulsion for alkaline seawater oxidation 基于氢键网络动态优化和静电斥力的碱性海水氧化协同抗氯性

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65100-5

Wei Zuo, Mingyu Liu, Shengjun Sun, Yu Yang, Zixiao Li, Xixi Zhang, Chaoxin Yang, Hefeng Wang, Imran Shakir, Xuefei Liu, Qian Liu, Xuping Sun, Bo Tang

{"title":"Synergistic chloride resistance via hydrogen−bond network dynamic optimization and electrostatic repulsion for alkaline seawater oxidation","authors":"Wei Zuo, Mingyu Liu, Shengjun Sun, Yu Yang, Zixiao Li, Xixi Zhang, Chaoxin Yang, Hefeng Wang, Imran Shakir, Xuefei Liu, Qian Liu, Xuping Sun, Bo Tang","doi":"10.1016/S1872-2067(26)65100-5","DOIUrl":"10.1016/S1872-2067(26)65100-5","url":null,"abstract":"<div><div>Seawater electrolysis, while promising for sustainable hydrogen production, is fundamentally challenged by the relentless chloride ions (Cl–)-induced corrosion, which impairs catalyst stability during long-term operation. We report a polyhydroquinone (PHQ)-modified electrocatalyst, where the redox-active PHQ layer is firmly coated to CoFe layered double hydroxide (CoFe LDH) surface through a strong hydrogen-bond network. Theoretical calculations and characterization techniques collectively elucidate that the unique interface creates an in situ protective coating, which effectively optimizes the composition of the interfacial water and prevents Cl– attack. Such a catalyst shows outstanding performance in alkaline seawater, requiring an overpotential of only 335 mV to reach 1 A cm–2 and exhibiting remarkable durability for 2000 h even at high current densities (j = 1, 1.5, and 2 A cm–2). Furthermore, the constructed alkaline anion exchange membrane water electrolyzer achieves a j of 1 A cm–2 at a low voltage of 2.55 V, significantly outperforming the benchmark Pt/C/NF||RuO2/NF.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 295-304"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651909","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

Decoding structure-selectivity interplay in Pd-Ag nanocatalysts for butadiene semi-hydrogenation 丁二烯半加氢钯银纳米催化剂结构-选择性相互作用的解码

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65078-4

Jiaxiang Qin, Songpei Zhang, Xingju Li, Xintai Chen, Jia Zhao, Xiaoling Mou, Xiangen Song, Li Yan, Ronghe Lin, Yunjie Ding

{"title":"Decoding structure-selectivity interplay in Pd-Ag nanocatalysts for butadiene semi-hydrogenation","authors":"Jiaxiang Qin, Songpei Zhang, Xingju Li, Xintai Chen, Jia Zhao, Xiaoling Mou, Xiangen Song, Li Yan, Ronghe Lin, Yunjie Ding","doi":"10.1016/S1872-2067(26)65078-4","DOIUrl":"10.1016/S1872-2067(26)65078-4","url":null,"abstract":"<div><div>Precise control over product selectivity in heterogeneous catalysis remains a key challenge due to the complex interplay of structural and electronic factors. Here, we demonstrate delicate tuning of product distribution in 1,3-butadiene semi-hydrogenation by engineering the size and composition of Pd-Ag nanostructures. By systematically decoupling size and electronic effects, we identify critical selectivity descriptors and establish structure-selectivity correlations across both monometallic and bimetallic series. The thresholds of ensemble size and Pd valence state for the formation of distinct products are experimentally determined. Integrating kinetic analysis, chemisorption studies, and density functional theory calculations, we show that increased ensemble size and Ag incorporation weaken 1-butene binding and elevate hydrogenation barriers, enabling selective formation of 1-butene (up to 66%) over thermodynamically favored 2-butenes. These insights reveal the fundamental roles of geometric and electronic modulation in governing selectivity and offer a generalizable framework for the rational design of multifunctional bimetallic catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 342-352"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148652129","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

Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H2O2 synthesis 三唑环功能化聚七嗪亚胺：利用供体-受体结构增强太阳能驱动的H2O2合成

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65093-0

Sue-Faye Ng, Joel Jie Foo, Karlo Nolkemper, Zahra Hajiahmadi, Jaya Bharti, Nannan Hou, Jiankang Zheng, Thomas D. Kühne, Markus Antonietti, Christian Mark Pelicano, Wee-Jun Ong

{"title":"Triazole ring functionalized poly(heptazine imide): Leveraging donor- acceptor configuration toward enhanced solar-driven H2O2 synthesis","authors":"Sue-Faye Ng, Joel Jie Foo, Karlo Nolkemper, Zahra Hajiahmadi, Jaya Bharti, Nannan Hou, Jiankang Zheng, Thomas D. Kühne, Markus Antonietti, Christian Mark Pelicano, Wee-Jun Ong","doi":"10.1016/S1872-2067(26)65093-0","DOIUrl":"10.1016/S1872-2067(26)65093-0","url":null,"abstract":"<div><div>Light-driven synthesis of hydrogen peroxide (H2O2) presents an ideal pathway for sustainability as compared to the traditional anthraquinone process. Herein, we introduce a strategic approach for functionalizing poly(heptazine imide) with triazole groups via a one-step calcination process using alkali-metal salts (NaCl/KCl/LiCl). Featuring a donor-acceptor framework that promotes singlet electron dissociation, the optimal catalyst (KNa) displayed outstanding photocatalytic performance, achieving H2O2 production at 9.32 mmol L–1 h–1 and benzaldehyde (BAD) generation at 8.14 mmol L–1 h–1. KNa reached an apparent quantum efficiency of 11.58% at 420 nm, in the absence of noble-metal cocatalysts. It also exhibited an electron-hole utilization close to unity (89%), indicating its efficiency in driving photoredox reactions. Mechanistic studies conducted through electrochemical measurements and scavenger tests revealed that KNa facilitated a 2-electron pathway for H2O2 production, with photogenerated charges and radicals (electron, hole, O2•–, 1O2) participating in the reaction. A shift in electron density and enhanced O2 adsorption observed from computational analysis reflects the donor-acceptor effect of the terminal triazole units on PHI. The versatility of KNa for other photochemical reactions was also exemplified by its simultaneous generation of H2O2 (1.11 mmol L–1 h–1) and furfuraldehyde (0.75 mmol L–1 h–1). As such, this research paves an in-depth understanding of synergistic dual-functional photocatalysts for photoredox reactions.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 140-155"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148660817","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

Regulation of Metal−Sulfur bond polarizability in Zn0.5Cd0.5S for visible-light-driven photocatalytic overall water splitting Zn0.5Cd0.5S中金属-硫键极化率对可见光光催化全水分解的调控

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65099-1

Chen Wang, Yue Zhang, Haolin Luo, Huoshuai Huang, Qianxiang Su, Zhen Ye, Zhi Jiang, Yong Zhu, Mingxia Chen, Zhidong Wei, Wenfeng Shangguan

{"title":"Regulation of Metal−Sulfur bond polarizability in Zn0.5Cd0.5S for visible-light-driven photocatalytic overall water splitting","authors":"Chen Wang, Yue Zhang, Haolin Luo, Huoshuai Huang, Qianxiang Su, Zhen Ye, Zhi Jiang, Yong Zhu, Mingxia Chen, Zhidong Wei, Wenfeng Shangguan","doi":"10.1016/S1872-2067(26)65099-1","DOIUrl":"10.1016/S1872-2067(26)65099-1","url":null,"abstract":"<div><div>The development of efficient and stable visible-light-driven Z-scheme systems for overall water splitting was crucial for solar hydrogen production. However, performance was often limited by photocorrosion of sulfide-based hydrogen evolution photocatalysts and competing, deactivating side reactions involving the redox shuttle. Herein, we construct a robust Z-scheme system by employing a CoP-modified Ni-doped Zn0.5Cd0.5S heterojunction with strong interfacial interaction as the HEP, coupled with BiVO4 as the oxygen evolution photocatalyst. The optimized system exhibited an apparent quantum yield of 4.06% at 420 nm and enabled sustained co-evolution of hydrogen and oxygen at a near-stoichiometric ratio. It also demonstrated outstanding cycling stability. Crucially, it had been demonstrated that the regulation of the internal polarizability of HEP effectively suppressed the competitive reduction of the redox medium and the formation of passivated Prussian blue derivatives on the catalyst surface. This work provides fundamental insights into mitigating the side effects caused by fusion through polarizability regulation.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 217-229"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651902","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

Local-atomic environment engineering of Ni-sites for industrial hydrogen production from seawater 工业海水制氢ni -site的局部原子环境工程

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65051-6

Pengfei Wu, Zhihao Lou, Yuanshuo Ma, Pengfei Wang, Da Xue, Fangyi Ma, Xuejing Cui, Guangbo Liu, Xin Zhou, Erdong Wang, Luhua Jiang

{"title":"Local-atomic environment engineering of Ni-sites for industrial hydrogen production from seawater","authors":"Pengfei Wu, Zhihao Lou, Yuanshuo Ma, Pengfei Wang, Da Xue, Fangyi Ma, Xuejing Cui, Guangbo Liu, Xin Zhou, Erdong Wang, Luhua Jiang","doi":"10.1016/S1872-2067(26)65051-6","DOIUrl":"10.1016/S1872-2067(26)65051-6","url":null,"abstract":"<div><div>Seawater electrolysis integrated with renewable energy sources represents a green and sustainable pathway for hydrogen production, yet its practical application is severely constrained by the lack of cost-effective, highly active, and scalable electrodes. Herein, we report the construction of a high-performance hydrogen evolution reaction (HER) electrode by engineering the local-atomic environment of Ni sites through vanadium oxide modification. This optimized electrode delivers current densities of 500/1000 mA cm–2 at only 283/361 mV in alkaline seawater. Impressively, a kW-scale alkaline seawater electrolyzer achieves continuous operation at an industrial-level current up to 25 A for over 880 h with an ultra-low degradation rate of 34.1 μV h–1. Combined experimental and theoretical investigations reveal a volcano-type relationship between the chemical state of Ni and the adsorption energy of the key intermediate H* (∆GH*), as well as the potential of zero charge (PZC) of the electrode. Furthermore, in-situ Fourier-transform infrared spectroscopy confirms that a lower PZC promotes the formation of more free water molecules near the electrode surface, thereby facilitating the HER process. This work uncovers atomic environment-governed HER mechanisms and develops a scalable, industrially stable seawater electrolysis electrode, bridging lab-innovation to practical hydrogen production.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 254-268"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148651905","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

Neighboring Ni-Cu dual single-atom sites regulate the local environment of interfacial water for promoting CO2 electroreduction kinetics in CO2-to-CO conversion 邻近的Ni-Cu双单原子位点调节界面水的局部环境，促进CO2-to- co转化中的CO2电还原动力学

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65092-9

Qi Hao, Qi Tang, Junxiu Wu, Kai Liu, Jun Lu, Tianpin Wu

{"title":"Neighboring Ni-Cu dual single-atom sites regulate the local environment of interfacial water for promoting CO2 electroreduction kinetics in CO2-to-CO conversion","authors":"Qi Hao, Qi Tang, Junxiu Wu, Kai Liu, Jun Lu, Tianpin Wu","doi":"10.1016/S1872-2067(26)65092-9","DOIUrl":"10.1016/S1872-2067(26)65092-9","url":null,"abstract":"<div><div>We develop a Ni-Cu dual single-atom catalyst (DSAC) as a model catalyst to investigate the neighboring synergy in dual single-atom sites for promoting the electrocatalytic carbon dioxide reduction reaction (ECO2RR) kinetics. Through detailed electrochemical tests, in situ spectroscopic observations and theoretical calculations, we found that during ECO2RR, the neighboring Ni-Cu dual single-atom sites synergistically weaken the rigidity of the hydrogen-bond networks of interfacial water and optimize the spatial configuration of water molecules surrounding the Ni-Cu dual single-atom sites, which increases the proportion of easily dissociated water species in the interfacial water, thus accelerating the CO2 protonation kinetics during the conversion of CO2 to CO. As a result, Ni-Cu DSAC exhibits a 1.5-fold increase and a 15-fold increase in ECO2RR activity compared to Ni SAC and Cu SAC, respectively. In flow cell electrolyzer, Ni-Cu DSAC achieves almost 100% Faradaic efficiency for CO production (FECO) from applied current density of 50 to 400 mA cm−2, with the optimal full-cell energy efficiency of 61.1% for CO production, reflecting the excellent catalytic performance of neighboring Ni-Cu dual single-atom sites for selective conversion of CO2 to CO. Benefiting from the efficient suppression of carbonates formation in acidic media, Ni-Cu DSAC achieves an outstanding single-pass carbon efficiency of 67.3% for CO2-to-CO conversion at 200 mA cm−2. Additionally, Ni-Cu DSAC also exhibits excellent long-term stability, with less than 10% decay of FECO throughout a 170-h continuous electrolysis in strong acid (pH = 1, j = 200 mA cm−2).</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 47-58"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148652095","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

Electron-deficient nickel tailored by boron for coke-free methane dry reforming 硼为无焦甲烷干重整量身定制的缺电子镍

IF 17.2 1区化学

Chinese Journal of Catalysis Pub Date : 2026-08-01 Epub Date: 2026-08-02 DOI: 10.1016/S1872-2067(26)65077-2

Yang Wang, Lei He, Fan Tang, Wen-Cui Li, Bowen He, Xi Liu, Liwei Chen, Dongqi Wang, Wenjie Shen, An-Hui Lu

{"title":"Electron-deficient nickel tailored by boron for coke-free methane dry reforming","authors":"Yang Wang, Lei He, Fan Tang, Wen-Cui Li, Bowen He, Xi Liu, Liwei Chen, Dongqi Wang, Wenjie Shen, An-Hui Lu","doi":"10.1016/S1872-2067(26)65077-2","DOIUrl":"10.1016/S1872-2067(26)65077-2","url":null,"abstract":"<div><div>Methane dry reforming (MDR) converts two major greenhouse gases (CO2 and CH4) into syngas (H2/CO) for synthesizing fuels and chemicals, which provides a process both economically viable and environmentally friendly, aligning with the goal of carbon neutrality. Ni is the most efficient and economic non-noble active metal for MDR but often suffers from deactivation caused by sintering or coking due to the fast C–H activation but sluggish carbon removal. Herein, we report a rather stable Ni catalyst (NiBN) derived from electrostatic-driven self-assembled 2D composites, which offered a coke-free manner for a prolonged stability (over 350 h) under typical MDR conditions. This outperformed catalyst featured with homogeneously distributed spherical Ni nanoparticles (~6 nm) stabilized within mixed-oxide matrix. Partially electron-deficient Ni species are tailored by surrounded boron species through the Ni–O–B structure, which hindered the last C–H bond cleavage of methane and accelerated CO2 reactivity, thus balancing elementary steps to enable a coke-free operation. It marks an important step forward for C–H bond manipulation and inspires material design in other applications.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"87 ","pages":"Pages 353-362"},"PeriodicalIF":17.2,"publicationDate":"2026-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148652130","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