Chinese Journal of Catalysis最新文献

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Ultrathin two-dimensional electrocatalysts: Structure-property relationships, mechanistic insights, and applications in water electrolysis 超薄二维电催化剂:结构-性质关系,机理见解,以及在水电解中的应用
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64783-8
Lina Wang , Muhan Na , Ruofei Du , Xiujin Wang , Boyang Yu , Lan Yang , Hui Chen , Xiaoxin Zou
{"title":"Ultrathin two-dimensional electrocatalysts: Structure-property relationships, mechanistic insights, and applications in water electrolysis","authors":"Lina Wang ,&nbsp;Muhan Na ,&nbsp;Ruofei Du ,&nbsp;Xiujin Wang ,&nbsp;Boyang Yu ,&nbsp;Lan Yang ,&nbsp;Hui Chen ,&nbsp;Xiaoxin Zou","doi":"10.1016/S1872-2067(25)64783-8","DOIUrl":"10.1016/S1872-2067(25)64783-8","url":null,"abstract":"<div><div>The pursuit of sustainable hydrogen production has positioned water electrolysis as a cornerstone technology for global carbon neutrality. However, sluggish kinetics, catalyst scarcity, and system integration challenges hinder its widespread deployment. Ultrathin two-dimensional (2D) materials, with their atomically exposed surfaces, tunable electronic structures, and defect-engineering capabilities, present unique opportunities for next-generation electrocatalysts. This review provides an integrated overview of ultrathin 2D electrocatalysts, discussing their structural diversity, synthetic routes, structure-activity relationships, and mechanistic understanding in water electrolysis processes. Special focus is placed on the translation of 2D materials from laboratory research to practical device implementation, emphasizing challenges such as scalable fabrication, interfacial engineering, and operational durability in realistic electrolyzer environments. The role of advanced characterization techniques in capturing dynamic structural changes and active site evolution is discussed. Finally, we outline future research directions, emphasizing the synergy of machine learning-driven materials discovery, advanced operando characterization, and scalable system integration to accelerate the industrial translation of 2D electrocatalysts for green hydrogen production.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 4-19"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060775","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 strong Pt-N3O coordination in graphene nanosheets accelerates the 4e− electrocatalytic oxygen reduction process 石墨烯纳米片中pt - n30o的强配位加速了4e−电催化氧还原过程
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64768-1
Xinqi Wang , Xueyuan Zhang , Menggai Jiao , Runlin Ma , Fang Xie , Hao Wan , Xiangjian Shen , Li-Li Zhang , Wei Ma , Zhen Zhou
{"title":"The strong Pt-N3O coordination in graphene nanosheets accelerates the 4e− electrocatalytic oxygen reduction process","authors":"Xinqi Wang ,&nbsp;Xueyuan Zhang ,&nbsp;Menggai Jiao ,&nbsp;Runlin Ma ,&nbsp;Fang Xie ,&nbsp;Hao Wan ,&nbsp;Xiangjian Shen ,&nbsp;Li-Li Zhang ,&nbsp;Wei Ma ,&nbsp;Zhen Zhou","doi":"10.1016/S1872-2067(25)64768-1","DOIUrl":"10.1016/S1872-2067(25)64768-1","url":null,"abstract":"<div><div>Single-metal sites anchored in nitrogen-doped nanocarbons are recognized as potent electrocatalysts for applications in energy conversion and storage. Here, an innovative inorganic salt-mediated secondary calcination strategy was developed to construct robust Pt single-atom catalysts on nitrogen- and oxygen-doped graphene nanosheets (Pt-N/O-GNs), thereby significantly enhancing the efficiency of the electrocatalytic oxygen reduction reaction (ORR). The ultrathin N/O-GNs, obtained by stripping Zn-ZIF with auxiliaries of KCl and LiCl, provide stable anchoring sites for highly exposed Pt-N<sub>3</sub>O active structures. The Pt-N/O-GNs catalyst, featuring a low Pt loading of 0.44 wt%, demonstrates exceptional mass activity in the ORR process. It attains an impressive onset potential of 0.99 V and a half-wave potential of 0.88 V. The zinc-air battery driven by the Pt-N/O-GNs displays superior power density and cycle stability. Theoretical computational studies reveal that the structure of heteroatoms doped in few-layer graphene facilitates the stable anchoring of single-atom configurations. The findings provide new perspectives for the tailored design and fabrication of single-metal-site electrocatalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 227-235"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145061245","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
Computational insights and strategic choices of nitrate and nitric oxide electroreduction to ammonia 硝酸和一氧化氮电还原制氨的计算见解和策略选择
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64776-0
Pu Guo , Shaoxue Yang , Huijuan Jing , Dong Luan , Jun Long , Jianping Xiao
{"title":"Computational insights and strategic choices of nitrate and nitric oxide electroreduction to ammonia","authors":"Pu Guo ,&nbsp;Shaoxue Yang ,&nbsp;Huijuan Jing ,&nbsp;Dong Luan ,&nbsp;Jun Long ,&nbsp;Jianping Xiao","doi":"10.1016/S1872-2067(25)64776-0","DOIUrl":"10.1016/S1872-2067(25)64776-0","url":null,"abstract":"<div><div>Electrochemical nitrate reduction (eNO<sub>3</sub>RR) and nitric oxide reduction (eNORR) to ammonia have emerged as promising and sustainable alternatives to the traditional Haber-Bosch method for ammonia production, particularly within the recently proposed reverse artificial nitrogen cycle route: N<sub>2</sub> → NO<sub><em>x</em></sub> → NH<sub>3</sub>. Notably, experimental studies have demonstrated that eNORR exhibits superior performance over eNO<sub>3</sub>RR on Cu<sub>6</sub>Sn<sub>5</sub> catalysts. However, the fundamental mechanisms underlying this difference remain poorly understood. Herein, we performed systematic theoretical calculations to explore the reaction pathways, electronic structure effects, and potential-dependent Faradic efficiency associated with ammonia production <em>via</em> these two distinct electrochemical pathways (eNORR and eNO<sub>3</sub>RR) on Cu<sub>6</sub>Sn<sub>5</sub>. By implementing an advanced ‘adaptive electric field controlled constant potential (EFC-CP)’ methodology combined with microkinetic modeling, we successfully reproduced the experimental observations and identified the key factors affecting ammonia production in both reaction pathways. It was found that eNORR outperforms eNO<sub>3</sub>RR because it circumvents the *NO<sub>2</sub> dissociation and *NO<sub>2</sub> desorption steps, leading to distinct surface coverage of key intermediates between the two pathways. Furthermore, the reaction rates were found to exhibit a pronounced dependence on the surface coverage of *NO in eNORR and *NO<sub>2</sub> in eNO<sub>3</sub>RR. Specifically, the facile desorption of *NO<sub>2</sub> on the Cu<sub>6</sub>Sn<sub>5</sub> surface in eNO<sub>3</sub>RR limits the attainable surface coverage of *NO, thereby impeding its performance. In contrast, the eNORR can maintain a high surface coverage of adsorbed *NO species, contributing to its enhanced ammonia production performance. These fundamental insights provide valuable guidance for the rational design of catalysts and the optimization of reaction routes, facilitating the development of more efficient, sustainable, and scalable techniques for ammonia production.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 220-226"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145061244","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 photocatalytic water oxidation via interfacial electric field-mediated charge separation in S-scheme photocatalyst s型光催化剂中界面电场介导的电荷分离促进光催化水氧化
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64757-7
Xinyue Tan , Minghui Zhang , Yang Bai , Xiaoyu Liu , Jianfang Jing , Yiguo Su
{"title":"Boosting photocatalytic water oxidation via interfacial electric field-mediated charge separation in S-scheme photocatalyst","authors":"Xinyue Tan ,&nbsp;Minghui Zhang ,&nbsp;Yang Bai ,&nbsp;Xiaoyu Liu ,&nbsp;Jianfang Jing ,&nbsp;Yiguo Su","doi":"10.1016/S1872-2067(25)64757-7","DOIUrl":"10.1016/S1872-2067(25)64757-7","url":null,"abstract":"<div><div>The major challenge in photocatalytic water splitting lies in water oxidation reactions, which still suffer from poor charge separation. This study overcame inefficient charge separation by establishing a robust interfacial electric field through the electrostatic-driven assembly of Co<sub>3</sub>O<sub>4</sub> nanoparticles with a perylene imide supramolecule (PDINH). The well-aligned band structures and intimate interfacial contact in the PDINH/Co<sub>3</sub>O<sub>4</sub> heterostructure create an enhanced interfacial electric field that is 4.1- and 53.2-fold stronger than those of individual PDINH and Co<sub>3</sub>O<sub>4</sub>, thus promoting directional charge separation and transfer. Moreover, S-scheme charge transfer strongly preserves the oxidative holes in PDINH to drive efficient water oxidation reactions. Consequently, PDINH/Co<sub>3</sub>O<sub>4</sub> composite achieves a photocatalytic oxygen evolution rate of 29.26 mmol g<sup>–1</sup> h<sup>–1</sup> under visible light irradiation, 8.2-fold improvement over pristine PDINH, with an apparent quantum yield of 6.66% at 420 nm. This study provides fundamental insights into interfacial electric field control for the development of high-performance organic photocatalysts for efficient water oxidation.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 199-209"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145061313","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
Simple removal of framework aluminum from MWW type zeolites for unprecedented optimal Mo-impregnated catalysts: Systematic elucidation of coke deposition and its impact on methane dehydroaromatization 从MWW型沸石中简单去除框架铝,获得前所未有的最佳mo浸渍催化剂:系统阐明焦炭沉积及其对甲烷脱氢芳构化的影响
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64760-7
Tristan James Sim , Yun Ha Song , Jaehee Shim , Gihoon Lee , Liangqing Li , Young Soo Ko , Jungkyu Choi
{"title":"Simple removal of framework aluminum from MWW type zeolites for unprecedented optimal Mo-impregnated catalysts: Systematic elucidation of coke deposition and its impact on methane dehydroaromatization","authors":"Tristan James Sim ,&nbsp;Yun Ha Song ,&nbsp;Jaehee Shim ,&nbsp;Gihoon Lee ,&nbsp;Liangqing Li ,&nbsp;Young Soo Ko ,&nbsp;Jungkyu Choi","doi":"10.1016/S1872-2067(25)64760-7","DOIUrl":"10.1016/S1872-2067(25)64760-7","url":null,"abstract":"<div><div>In this study, we investigated Mo-impregnated H-MCM-22 catalysts (denoted Mo/M) for methane dehydroaromatization (MDA) to produce aromatics such as benzene and toluene (BT). We attempted to improve the performance of the MDA catalysts by reducing the amount of Brönsted acid sites (BAS) of the H-MCM-22 supports via hydrothermal dealumination. Among the prepared catalysts, an optimal hydrothermal treatment (HT) of H-MCM-22 supports at 400 °C, followed by Mo impregnation (denoted Mo/M_400), resulted in a reduced and optimal amount of BAS, along with a comparable Mo distribution to Mo/M. Further, Mo/M_400 enhanced BT formation rates (maximum BT formation rate of 5.23 <em>vs</em>. 4.73 mmol<sub>BT</sub>·g<sup>−1</sup>·h<sup>−1</sup> for Mo/M); it appears that dealumination-induced reduction in the quantity of BAS altered their spatial interaction with active Mo species, promoting BT and naphthalene formation. Interestingly, the lifetime of intermediate C<sub>2</sub> (ethane and ethylene) formation was also improved for Mo/M_400. Rigorous coke analyses revealed that the decreased coke content in the aromatic-selective 10-membered-ring (10-MR) pores, as well as the ability of the 12-MR pores to accommodate coke deposits over a longer reaction time, improved the stability of Mo/M_400. Nonetheless, for all catalysts, the deactivations of BAS, and subsequently, the active Mo sites were mainly ascribed to coke deposition. The overall enhancement in MDA performance by Mo/M_400 was attributed to the advantages of the optimally reduced BAS, allowing such performance to surpass those of previously reported Mo-based catalysts.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 123-143"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060728","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
Asymmetric synthesis of chiral N-substituted amino amides and esters with two chiral centers by imine reductase-catalyzed dynamic kinetic resolution via reductive amination 亚胺还原酶催化还原胺化动力学拆分不对称合成手性n取代氨基酰胺及双手性中心酯
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64769-3
Zefei Xu , Jinhui Feng , Xiangtao Liu , Qian Li , Weidong Liu , Peiyuan Yao , Qiaqing Wu , Dunming Zhu
{"title":"Asymmetric synthesis of chiral N-substituted amino amides and esters with two chiral centers by imine reductase-catalyzed dynamic kinetic resolution via reductive amination","authors":"Zefei Xu ,&nbsp;Jinhui Feng ,&nbsp;Xiangtao Liu ,&nbsp;Qian Li ,&nbsp;Weidong Liu ,&nbsp;Peiyuan Yao ,&nbsp;Qiaqing Wu ,&nbsp;Dunming Zhu","doi":"10.1016/S1872-2067(25)64769-3","DOIUrl":"10.1016/S1872-2067(25)64769-3","url":null,"abstract":"<div><div>Chiral <em>N</em>-substituted amino amides and esters are ubiquitous scaffolds in pesticides and pharmaceutical chemicals, but their asymmetric synthesis remains challenging especially for those with multiple chiral centers. In this study, IR104 from <em>Streptomyces aureocirculatus</em> was identified from 157 wild-type imine reductases for the synthesis of (<em>S</em>)-2-((<em>R</em>)-2-oxo-4-propylpyrrolidin-1-yl) butanamide (antiepileptic drug Brivaracetam) via dynamic kinetic resolution reductive amination from ethyl 3-formylhexanoate and (<em>S</em>)-2-aminobutylamide with high diastereoselectivity. To further improve the catalytic efficiency of IR104, its mutant D191E/L195I/E253S/M258A (M3) was identified by saturation mutagenesis and iterative combinatorial mutagenesis, which exhibited a 102-fold increase in the catalytic efficiency relative to that of wild-type enzyme and high diastereoselectivity (98:2 <em>d.r.</em>). Crystal structural analysis and molecular dynamics simulations provided some insights into the molecular basis for the improved activity of the mutant enzyme. The imine reductase identified in this study could accept chiral amino amides/esters as amino donors for the dynamic kinetic resolution reductive amination of racemic <em>α</em>-substituted aldehydo-esters, expanding the substrate scope of imine reductases in the dynamic kinetic resolution-reductive amination. Finally, IR104-M3 was successfully used for the preparation of Brivaracetam at gram scale. Using this mutant, various <em>N</em>-substituted amino amides/esters with two chiral centers were also synthesized with up to 99:1 <em>d.r.</em> and 96% yields and subsequently converted into γ- and δ-lactams, providing an efficient protocol for the synthesis of these important compounds via enzymatic dynamic kinetic resolution-reductive amination from simple building blocks.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 144-152"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060729","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
Electronic structure modulation of metal based organic catalysts for photocatalytic H2O2 production 光催化生产H2O2的金属基有机催化剂的电子结构调制
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64788-7
Wenhui Qi , Xiuyan Li , Shaonan Gu , Bin Sun , Yinan Wang , Guowei Zhou
{"title":"Electronic structure modulation of metal based organic catalysts for photocatalytic H2O2 production","authors":"Wenhui Qi ,&nbsp;Xiuyan Li ,&nbsp;Shaonan Gu ,&nbsp;Bin Sun ,&nbsp;Yinan Wang ,&nbsp;Guowei Zhou","doi":"10.1016/S1872-2067(25)64788-7","DOIUrl":"10.1016/S1872-2067(25)64788-7","url":null,"abstract":"<div><div>Photocatalytic synthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) has emerged as a promising approach because of its simplicity and environmental benefits. However, significant challenges remain obstacles to their advancement, such as the rapid recombination of photogenerated charge carriers and sluggish surface redox reactions on nonmetallic organic catalysts. Metal-based organic catalysts with tunable electronic structures are considered ideal for exploring the mechanisms and structure-performance relationships in H<sub>2</sub>O<sub>2</sub> synthesis. This review summarizes the fundamental principles of photocatalytic H<sub>2</sub>O<sub>2</sub> synthesis <em>via</em> oxygen reduction and water oxidation reactions. Recent advancements in electronic structure tuning strategies for metal-based organic catalysts are critically examined, focusing on their impact on light absorption range, photogenerated carrier separation, O<sub>2</sub> activation, and the selective generation of H<sub>2</sub>O<sub>2</sub>. In addition, this review comprehensively evaluates the applications of sacrificial agents in photocatalytic reaction systems and offers insights into the future development of metal-based organic catalysts for H<sub>2</sub>O<sub>2</sub> photosynthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 45-69"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145060779","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 spin polarization of encaging Co nanoparticles in atomic CoNx sites evoke high valent Co species for boosting organic compound oxidation 工程自旋极化包裹Co纳米粒子在原子的凸位激发高价Co,促进有机化合物氧化
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-09-15 DOI: 10.1016/S1872-2067(25)64763-2
Liang Zhang , Jialiang Rui , Yiqian Li , Zhizhi Yang , Shiro Kubuki , Junhu Wang , Bofan Zhang
{"title":"Engineering spin polarization of encaging Co nanoparticles in atomic CoNx sites evoke high valent Co species for boosting organic compound oxidation","authors":"Liang Zhang ,&nbsp;Jialiang Rui ,&nbsp;Yiqian Li ,&nbsp;Zhizhi Yang ,&nbsp;Shiro Kubuki ,&nbsp;Junhu Wang ,&nbsp;Bofan Zhang","doi":"10.1016/S1872-2067(25)64763-2","DOIUrl":"10.1016/S1872-2067(25)64763-2","url":null,"abstract":"<div><div>Precise manipulation of the catalytic spin configuration and delineation of the relationship between spin related properties and oxidation pathways remain significant challenges in Fenton-like processes. Herein, encapsulated cobalt nanoparticles and cobalt-nitrogen-doped carbon moieties, endowed with confinement effects and variations in shell curvature were constructed <em>via</em> straightforward pyrolysis strategies, inducing alterations in magnetic anisotropy, electronic energy levels and spin polarization. The enhanced spin polarization at cobalt sites leads to a reduction in crystal field splitting energy and an increase in electronic spin density. This phenomenon facilitated electron transfer from cobalt orbitals to <em>p</em><sub>z</sub> orbitals of oxygen species within peroxymonosulfate molecules, thereby promoting the formation of high-valent cobalt species. The encapsulation effectively stabilized cobalt nanoparticles, mitigating their dissolution or deactivation during reactions, which in turn enhances stability and durability in continuous flow processes. The high-valent cobalt species within the shell exhibit increased exposure and generate localized high concentrations, thereby intensifying interactions with migrating pollutants and enabling efficient and selective oxidation of emerging compounds with elevated redox potentials. This work underscores the profound impact of confined encapsulation curvature and spin polarization characteristics of metal sites on catalytic oxidation pathways and performance, opening novel avenues for spin engineering in practical environmental catalysis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"77 ","pages":"Pages 184-198"},"PeriodicalIF":17.7,"publicationDate":"2025-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145061312","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
Modulating electronic structure of g-C3N4 hosted Co-N4 active sites by axial phosphorus coordination for efficient overall H2O2 photosynthesis from oxygen and water 通过轴向磷配位调节g-C3N4承载Co-N4活性位点的电子结构,促进氧气和水对H2O2的有效整体光合作用
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-08-25 DOI: 10.1016/S1872-2067(25)64735-8
Shinuo Liang, Fengjun Li, Fei Huang, Xinyu Wang, Shengwei Liu
{"title":"Modulating electronic structure of g-C3N4 hosted Co-N4 active sites by axial phosphorus coordination for efficient overall H2O2 photosynthesis from oxygen and water","authors":"Shinuo Liang,&nbsp;Fengjun Li,&nbsp;Fei Huang,&nbsp;Xinyu Wang,&nbsp;Shengwei Liu","doi":"10.1016/S1872-2067(25)64735-8","DOIUrl":"10.1016/S1872-2067(25)64735-8","url":null,"abstract":"<div><div>Single-atom catalysts are promising for H<sub>2</sub>O<sub>2</sub> photosynthesis from O<sub>2</sub> and H<sub>2</sub>O, but their efficiency is still limited by the ill-defined electronic structure. In this study, Co single-atoms with unique four planar N-coordination and one axial P-coordination (Co-N<sub>4</sub>P<sub>1</sub>) are decorated on the lateral edges of nanorod-like crystalline g-C<sub>3</sub>N<sub>4</sub> (CCN) photocatalysts. Significantly, the electronic structures of central Co as active sites for O<sub>2</sub> reduction reaction (ORR) and planar N-coordinator as active sites for H<sub>2</sub>O oxidation reaction (WOR) in Co-N<sub>4</sub>P<sub>1</sub> can be well regulated by the synergetic effects of introducing axial P-coordinator, in contrast to the decorated Co single-atoms with only four planar N-coordination (Co-N<sub>4</sub>). Specifically, directional photoelectron accumulation at central Co active sites, induced by an introduced midgap level in Co-N<sub>4</sub>P<sub>1</sub>, mediates the ORR active sites from 4e<sup>–</sup>-ORR-selective terminal –NH<sub>2</sub> sites to 2e<sup>–</sup>-ORR-selective Co sites, moreover, an elevated d-band center of Co 3<em>d</em> orbital strengthens ORR intermediate *OOH adsorption, thus jointly facilitating a highly selective and active 2e<sup>–</sup>-ORR pathway to H<sub>2</sub>O<sub>2</sub> photosynthesis. Simultaneously, a downshifted p-band center of N 2<em>p</em> orbital in Co-N<sub>4</sub>P<sub>1</sub> weakens WOR intermediate *OH adsorption, thus enabling a preferable 2e<sup>–</sup>-WOR pathway toward H<sub>2</sub>O<sub>2</sub> photosynthesis. Subsequently, Co-N<sub>4</sub>P<sub>1</sub> exhibits exceptional H<sub>2</sub>O<sub>2</sub> photosynthesis efficiency, reaching 295.6 μmol g<sup>–1</sup> h<sup>–1</sup> with a remarkable solar-to-chemical conversion efficiency of 0.32 %, which is 15 times that of Co-N<sub>4</sub> (19.2 μmol g<sup>–1</sup> h<sup>–1</sup>) and 10 times higher than CCN (27.6 μmol g<sup>–1</sup> h<sup>–1</sup>). This electronic structure modulation on single-atom catalysts offers a promising strategy for boosting the activity and selectivity of H<sub>2</sub>O<sub>2</sub> photosynthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"76 ","pages":"Pages 81-95"},"PeriodicalIF":17.7,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144895852","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 progress in functional carbon-based materials for advanced electrocatalysis 先进电催化用功能碳基材料研究进展
IF 17.7 1区 化学
Chinese Journal of Catalysis Pub Date : 2025-08-25 DOI: 10.1016/S1872-2067(25)64749-8
Yinglong Weng , Jianping Zhang , Kun Zhang , Yitong Lu , Tingting Huang , Yingbo Kang , Xiaotong Han , Jieshan Qiu
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