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Carbon-supported platinum-based electrocatalysts for alkaline hydrogen evolution 碳负载铂基碱性析氢电催化剂
EES catalysis Pub Date : 2025-07-18 DOI: 10.1039/D5EY00147A
Qiuyue Yang, Jilan Zeng, Guowei Yang, Xinran Sun, Xiahui Lin, Kunlong Liu, Jiayi Chen, Sibo Wang and Xue Feng Lu
{"title":"Carbon-supported platinum-based electrocatalysts for alkaline hydrogen evolution","authors":"Qiuyue Yang, Jilan Zeng, Guowei Yang, Xinran Sun, Xiahui Lin, Kunlong Liu, Jiayi Chen, Sibo Wang and Xue Feng Lu","doi":"10.1039/D5EY00147A","DOIUrl":"https://doi.org/10.1039/D5EY00147A","url":null,"abstract":"<p >Water electrolysis hydrogen production technology directly generates high-purity hydrogen through electrochemical water splitting, serving as a key technology for achieving zero-carbon emission hydrogen production. Alkaline water electrolysis demonstrates marked advantages in efficiency and rapidly developing anode catalysts in an alkaline medium. Nevertheless, the sluggish kinetics of the hydrogen evolution reaction (HER) at the cathode in an alkaline environment constitute a fundamental bottleneck that restricts the extensive application of this technology. Platinum, serving as the benchmark catalyst for the HER, is limited in its large-scale development due to its scarcity and high cost. In comparison, carbon-supported platinum-based catalysts exhibit exceptional HER catalytic activity and stability, driven by their unique electronic architecture and the synergistic effect with the support. In this review, we comprehensively examine the latest progress of carbon-supported platinum-based materials for the alkaline HER, summarize the factors contributing to the slow kinetics of the HER in an alkaline environment, and then focus on the strategies for modifying the carbon substrate and synthesizing carbon-supported platinum-based nanomaterials. Finally, the review critically evaluates existing challenges and proposes targeted research directions to advance Pt-based electrocatalysts for practical alkaline hydrogen evolution systems.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 972-993"},"PeriodicalIF":0.0,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00147a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990362","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Plasma-driven redox mechanism in the reverse water–gas shift reaction over Ni–In intermetallic catalysts† Ni-In金属间催化剂上逆水气转换反应的等离子体驱动氧化还原机制
EES catalysis Pub Date : 2025-07-17 DOI: 10.1039/D5EY00101C
Dae-Yeong Kim, Zhang Wenjun, Kaiyue Dong, Bang Lu, Duanxing Li, Satoru Takakusagi, Shinya Furukawa and Tomohiro Nozaki
{"title":"Plasma-driven redox mechanism in the reverse water–gas shift reaction over Ni–In intermetallic catalysts†","authors":"Dae-Yeong Kim, Zhang Wenjun, Kaiyue Dong, Bang Lu, Duanxing Li, Satoru Takakusagi, Shinya Furukawa and Tomohiro Nozaki","doi":"10.1039/D5EY00101C","DOIUrl":"https://doi.org/10.1039/D5EY00101C","url":null,"abstract":"<p >The reverse water–gas shift (RWGS) reaction has been recognized as a promising strategy for CO<small><sub>2</sub></small> valorization. However, it faces limitations due to low activity and poor CO selectivity at low temperatures. In this study, we report that plasma can effectively promote the low-temperature RWGS reaction over Ni–In intermetallic catalysts. The formation of the Ni–In intermetallic phases completely suppresses CH<small><sub>4</sub></small> formation and achieves 100% CO selectivity. Through <em>in situ</em> transmission infrared spectroscopy (TIR) and <em>in situ</em> X-ray absorption fine-structure (XAFS) analysis, we monitored the changes occurring on the catalyst surface during the plasma reaction. The interaction between redox-active sites present in the Ni–In intermetallic catalysts and plasma-activated species lowers the activation energy, thereby facilitating the RWGS reaction at low temperatures. This study offers fundamental insights into how plasma-activated species enhance catalysis and the underlying mechanisms of low-temperature activation in plasma catalysis.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1098-1105"},"PeriodicalIF":0.0,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00101c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990341","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Alkali-cation-free electrochemical CO2 reduction to multicarbon products in aqueous electrolytes containing tetraalkylammonium cations† 含四烷基铵阳离子的水溶液中无碱阳离子电化学CO2还原多碳产物
EES catalysis Pub Date : 2025-07-04 DOI: 10.1039/D5EY00141B
Ryo Kurihara, Shotaro Ito, Shintaro Kato, Takashi Harada, Shuji Nakanishi and Kazuhide Kamiya
{"title":"Alkali-cation-free electrochemical CO2 reduction to multicarbon products in aqueous electrolytes containing tetraalkylammonium cations†","authors":"Ryo Kurihara, Shotaro Ito, Shintaro Kato, Takashi Harada, Shuji Nakanishi and Kazuhide Kamiya","doi":"10.1039/D5EY00141B","DOIUrl":"https://doi.org/10.1039/D5EY00141B","url":null,"abstract":"<p >The electrochemical reduction of CO<small><sub>2</sub></small> to multicarbon (C<small><sub>2+</sub></small>) products is attracting attention for the sustainable production of fuel and chemicals. Conventionally, electrolytes containing alkali cations are typically used; however, salt precipitation associated with these cations often hinders stable CO<small><sub>2</sub></small> electrolysis. Organic cations are promising alternatives to alkali cations. Herein, we conducted gaseous CO<small><sub>2</sub></small> electrolysis in aqueous solutions containing tetraalkylammonium cations in the absence of alkali cations to evaluate the effect of organic cations on C<small><sub>2+</sub></small> formation. When tetramethylammonium cations were present as the only cation species besides protons, the faradaic efficiency for CO<small><sub>2</sub></small> reduction exceeded 89% across a broad current density range of 0.1–1 A cm<small><sup>−2</sup></small>. In particular, C<small><sub>2+</sub></small> formation was efficient under high total current density conditions, reaching a faradaic efficiency of 69.6% and a partial current density of 0.7 A cm<small><sup>−2</sup></small>. By contrast, the use of larger cations such as tetraethylammonium and tetrapropylammonium cations resulted in lower ethylene selectivity. Numerical simulations based on the generalized modified Poisson–Nernst–Planck model suggested that the size of the tetraalkylammonium cations affects the electric field strength within the electric double layer, with smaller cations forming a stronger field that promotes ethylene formation.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1055-1061"},"PeriodicalIF":0.0,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00141b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990337","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unlocking the potential: key roles of interfacial water in electrocatalysis 释放潜力:界面水在电催化中的关键作用
EES catalysis Pub Date : 2025-07-01 DOI: 10.1039/D5EY00161G
Zheng Tang, Zhongliang Dong, Lingjie Yuan, Bowen Li and Yinlong Zhu
{"title":"Unlocking the potential: key roles of interfacial water in electrocatalysis","authors":"Zheng Tang, Zhongliang Dong, Lingjie Yuan, Bowen Li and Yinlong Zhu","doi":"10.1039/D5EY00161G","DOIUrl":"https://doi.org/10.1039/D5EY00161G","url":null,"abstract":"<p >Interfacial water, serving as a subtle yet powerful performance modulator, plays a pivotal role in various electrochemical technologies due to its unique configurations and dynamic properties. Especially in the past decade, advances in electrocatalyst research, experimental characterization and theoretical modeling have significantly deepened the understanding of interfacial water's role in electrocatalytic systems. These as-obtained insights not only elucidate the dynamic behavior and structural properties of interfacial water but also highlight its importance in optimizing reaction pathways and improving electrocatalytic performance. Therefore, the understanding and regulation of interfacial water is an important topic in electrocatalytic research, and motivated us to compile this review. This review starts with a thorough analysis of interfacial water's properties and behaviors relevant to the electrocatalysis including structural types, water networks, rigidity and molecular orientation. Then, the specific roles of interfacial water in electrocatalysis are subsequently analyzed and classified as a co-catalyst, a masking agent, a regulator of reaction intermediates, and an inducer of catalyst reconfiguration. Next, some advanced experimental characterization and computational methods are presented to collectively probe the interfacial water, which is critical to capture accurate structural information. Furthermore, we present a comprehensive overview of key strategies for modulating the properties and behaviors of interfacial water to enhance the electrocatalytic performance of representative reactions at the electrolyte and catalyst levels, with emphasis on the specific mechanisms behind these modulation approaches. Finally, we discuss current challenges and future opportunities in this field, aiming to inspire the design of more advanced electrocatalytic systems.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 943-971"},"PeriodicalIF":0.0,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00161g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Introduction to understanding and new approaches to create synergy between catalysis and plasma themed collection 介绍在催化和等离子体主题收集之间创造协同作用的理解和新方法
EES catalysis Pub Date : 2025-06-26 DOI: 10.1039/D5EY90015H
Annemie Bogaerts, Gabriele Centi and Jason C. Hicks
{"title":"Introduction to understanding and new approaches to create synergy between catalysis and plasma themed collection","authors":"Annemie Bogaerts, Gabriele Centi and Jason C. Hicks","doi":"10.1039/D5EY90015H","DOIUrl":"https://doi.org/10.1039/D5EY90015H","url":null,"abstract":"<p >A graphical abstract is available for this content</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 4","pages":" 592-594"},"PeriodicalIF":0.0,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey90015h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144536766","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Furfural electrovalorisation to hydrofuroin with near-unity faradaic efficiency on a single-atom zinc catalyst† 在单原子锌催化剂上以接近统一的法拉第效率将糠醛电价化为氢呋喃
EES catalysis Pub Date : 2025-06-23 DOI: 10.1039/D5EY00113G
Jiaxiang Chen, Songbo Ye, Fangxin She, Xin Yang, Fangzhou Liu, Zixun Yu, Zhi Zheng, Ming Hong, Qiang Wang, Yuan Chen, Hao Li and Li Wei
{"title":"Furfural electrovalorisation to hydrofuroin with near-unity faradaic efficiency on a single-atom zinc catalyst†","authors":"Jiaxiang Chen, Songbo Ye, Fangxin She, Xin Yang, Fangzhou Liu, Zixun Yu, Zhi Zheng, Ming Hong, Qiang Wang, Yuan Chen, Hao Li and Li Wei","doi":"10.1039/D5EY00113G","DOIUrl":"https://doi.org/10.1039/D5EY00113G","url":null,"abstract":"<p >Electrochemical valorisation of biomass to value-added chemical feedstocks holds great potential to reduce the reliance on fossil fuels and accelerate the realisation of a sustainable future. In this work, we show that hydrofuroin, an important feedstock for sustainable aviation fuels, can be selectively produced on a zinc (Zn) single-atom catalyst <em>via</em> the electrochemical furfural reduction reaction (FRR). Initial theoretical results show that the weak binding capability of a zinc (Zn) single-atom active center effectively suppresses the parasitic hydrogen evolution reaction (HER) while enabling fast desorption and dimerization of furfural radicals towards hydrofuroin formation, which was proved by our experimental validation. The catalyst, obtained by depositing zinc phthalocyanine on purified multi-walled carbon nanotubes, exhibits near-unity faradaic efficiency for hydrofuroin production in a wide potential window, <em>e.g.</em>, −0.5 to −0.8 V<small><sub>RHE</sub></small>. The kinetic study further provides mechanistic insights into hydrofuroin formation on the single-atom site. This catalyst can be integrated into a flow cell electrolyser to achieve highly efficient furfural conversion to sustainable fuel precursors, which is beneficial for biomass electrovalorisation to value-added green products and chemicals.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1062-1074"},"PeriodicalIF":0.0,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00113g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Inhibiting overoxidation of an α-MnO2 electrocatalyst by the lattice strain effect for efficient water oxidation† 通过晶格应变效应抑制α-MnO2电催化剂的过氧化,实现高效水氧化
EES catalysis Pub Date : 2025-06-23 DOI: 10.1039/D5EY00106D
Fang-Yi Li, Shan Guan, Jianming Liu, Changhao Liu, Junfeng Zhang, Ju Gu, Zhaosheng Li, Zhigang Zou and Zhen-Tao Yu
{"title":"Inhibiting overoxidation of an α-MnO2 electrocatalyst by the lattice strain effect for efficient water oxidation†","authors":"Fang-Yi Li, Shan Guan, Jianming Liu, Changhao Liu, Junfeng Zhang, Ju Gu, Zhaosheng Li, Zhigang Zou and Zhen-Tao Yu","doi":"10.1039/D5EY00106D","DOIUrl":"https://doi.org/10.1039/D5EY00106D","url":null,"abstract":"<p >The development of low-cost transition metal catalysts for use in alkaline water electrolysis (AWE) at high current densities is essential for achieving high-performance water splitting. Here, we reported a CrSb–MnO<small><sub>2</sub></small> catalyst, which shows a low overpotential of 263 mV at 100 mA cm<small><sup>−2</sup></small> and outstanding stability with only a small degradation of the catalyst after 100 h of operation at 1 A cm<small><sup>−2</sup></small> (1 M KOH). In addition, the catalyst also achieved excellent performance in AWE (1.69 V@1 A cm<small><sup>−2</sup></small>). This enhanced performance is not only due to lattice-strain engineering, which effectively modulates the electronic configurations of the active sites, but also due to bimetallic synergy, which improves the dynamics of metal–metal charge transfer. <em>In situ</em> differential electrochemical mass spectrometry (DEMS) and Fourier-transform infrared (FTIR) analyses revealed that the CrSb–MnO<small><sub>2</sub></small> catalyst preferred the adsorbate evolution mechanism (AEM) during the alkaline OER. This preference contributes to sustained stability under high current conditions in alkaline media. This work offers a novel approach for designing membrane electrodes that can operate efficiently and stably under large currents.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1134-1144"},"PeriodicalIF":0.0,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00106d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Outstanding Reviewers for EES Catalysis in 2024 2024年EES Catalysis优秀审稿人
EES catalysis Pub Date : 2025-06-18 DOI: 10.1039/D5EY90014J
{"title":"Outstanding Reviewers for EES Catalysis in 2024","authors":"","doi":"10.1039/D5EY90014J","DOIUrl":"https://doi.org/10.1039/D5EY90014J","url":null,"abstract":"<p >We would like to take this opportunity to thank all of <em>EES Catalysis</em>’s reviewers for helping to preserve quality and integrity in chemical science literature. We would also like to highlight the Outstanding Reviewers for <em>EES Catalysis</em> in 2024.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 882-882"},"PeriodicalIF":0.0,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey90014j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990348","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Spontaneous generation of an atomically dispersed Mo and MoS2 coupling catalyst via reaction induction transformation for enhancing local hydrogen concentration in hydrogenation† 通过反应诱导转化自发生成原子分散的Mo和MoS2偶联催化剂,提高加氢过程中局部氢浓度
EES catalysis Pub Date : 2025-06-17 DOI: 10.1039/D5EY00086F
Guangxun Sun, Peng Xue, Changle Yue, Yang Li, Hongfu Shi, Xin Zhang, Fengyu Tian, Junxi Li, Zekun Guan, Bin Liu, Zhi Liu, Yunqi Liu and Yuan Pan
{"title":"Spontaneous generation of an atomically dispersed Mo and MoS2 coupling catalyst via reaction induction transformation for enhancing local hydrogen concentration in hydrogenation†","authors":"Guangxun Sun, Peng Xue, Changle Yue, Yang Li, Hongfu Shi, Xin Zhang, Fengyu Tian, Junxi Li, Zekun Guan, Bin Liu, Zhi Liu, Yunqi Liu and Yuan Pan","doi":"10.1039/D5EY00086F","DOIUrl":"https://doi.org/10.1039/D5EY00086F","url":null,"abstract":"<p >The development of a synergistic coupling catalyst at the atomic scale for slurry-phase hydrogenation of vacuum residue (VR) is extremely challenging. Herein, we designed and constructed a robust coupling catalyst comprising Mo single atoms and MoS<small><sub>2</sub></small> (Mo SAs–MoS<small><sub>2</sub></small>) using a reaction induction transformation strategy. The spontaneous generation of Mo SAs–MoS<small><sub>2</sub></small> synergistically promoted H<small><sub>2</sub></small> activation and enhanced local active hydrogen concentration in the hydrogenation of VR. Benefiting from the strong hydrogen concentration distribution in MoS<small><sub>2</sub></small> and Mo SAs, the catalyst revealed remarkable hydrogenation performance toward VR with a TOF<small><sub>T</sub></small> of up to 0.39 s<small><sup>−1</sup></small>, liquid product yield of 92 wt%, and coke content of 0.6 wt%. Theoretical calculations revealed that the synergistic action of Mo SAs–MoS<small><sub>2</sub></small> facilitated electron transfer between Mo species and reactants, reducing the desorption energy barriers for H<small><sub>2</sub></small> and anthracene and thereby promoting the hydrogenation of VR. This work provides a novel idea for the design of efficient coupling catalysts for strengthening local active hydrogen concentration in the hydrogenation of VR, and this concept can be applied to other hydrogenation systems.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1145-1154"},"PeriodicalIF":0.0,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00086f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990346","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Atom-economical insertion of hydrogen and sulfur into carbon–nitrogen triple bonds using H2S via synergistic C–N sites† 利用H2S通过协同C-N位点将氢和硫原子经济地插入碳氮三键†
EES catalysis Pub Date : 2025-06-16 DOI: 10.1039/D5EY00110B
Ganchang Lei, Jiayin Wang, Xinhui Liu, Shiping Wang, Shijing Liang, Lijuan Shen, Yingying Zhan and Lilong Jiang
{"title":"Atom-economical insertion of hydrogen and sulfur into carbon–nitrogen triple bonds using H2S via synergistic C–N sites†","authors":"Ganchang Lei, Jiayin Wang, Xinhui Liu, Shiping Wang, Shijing Liang, Lijuan Shen, Yingying Zhan and Lilong Jiang","doi":"10.1039/D5EY00110B","DOIUrl":"https://doi.org/10.1039/D5EY00110B","url":null,"abstract":"<p >Developing efficient strategies that convert industrial waste hydrogen sulfide (H<small><sub>2</sub></small>S) into value-added products is meaningful for both applied environmental science and industrial chemistry. Here we report a series of heterogeneous N-doped carbon catalysts with synergistic C–N sites that enable the nucleophilic addition of H<small><sub>2</sub></small>S into aromatic nitrile compounds (PhCN) under mild conditions to produce thiobenzamide (PhCSNH<small><sub>2</sub></small>). The as-designed C–N sites achieve a high thioamide production rate of 26 400 μmol<small><sub>PhCSNH<small><sub>2</sub></small></sub></small> L<small><sup>−1</sup></small> h<small><sup>−1</sup></small> and a notable selectivity of <em>ca.</em> 80% at 60 °C within a short 2-hour timeframe. Additionally, the catalyst exhibits easy recyclability and maintains high stability over ten cycles during a 6-month period. Systematic microscopic and <em>in situ</em> spectroscopic characterization, combined with theoretical calculations, reveal that C-pyridinic N coordination sites effectively lower the adsorption energy barrier of the crucial intermediate *PhCSHNH, offering a dynamically favorable pathway for PhCSNH<small><sub>2</sub></small> production. Furthermore, the protocol demonstrates excellent compatibility with various substituted substrates, providing access to a diverse range of thioamides.</p>","PeriodicalId":72877,"journal":{"name":"EES catalysis","volume":" 5","pages":" 1106-1116"},"PeriodicalIF":0.0,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ey/d5ey00110b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144990342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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