Chinese Journal of Catalysis最新文献_第8页

Ultrafast electron transfer in 2D/2D g-C3N4/WO3 S-scheme heterojunctions for enhanced H2O2 production 2D/2D g-C3N4/WO3 S-scheme异质结中超快电子转移增强H2O2生成

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)64949-2

Ping Li , Liang Wei , Wei Xia , Chengcheng Yuan , Chenbin Ai , Meng Li

{"title":"Ultrafast electron transfer in 2D/2D g-C3N4/WO3 S-scheme heterojunctions for enhanced H2O2 production","authors":"Ping Li , Liang Wei , Wei Xia , Chengcheng Yuan , Chenbin Ai , Meng Li","doi":"10.1016/S1872-2067(26)64949-2","DOIUrl":"10.1016/S1872-2067(26)64949-2","url":null,"abstract":"<div><div>The increasing demand for sustainable and environmentally friendly hydrogen peroxide (H2O2) production has necessitated the development of efficient photocatalytic strategies. A two-dimensional (2D)/2D graphitic carbon nitride (g-C3N4)/WO3 S-scheme heterojunction was synthesized in this study via in situ growth, yielding an atomically intimate interface that promotes ultrafast interfacial charge transfer. Comprehensive spectroscopy, photoelectrochemistry, Kelvin probe force microscopy, and density functional theory investigations confirmed the S-scheme charge-transfer mechanism. This system, driven by an internal electric field, promotes the spatial separation of photoexcited charge carriers and maintains robust redox abilities. Femtosecond transient absorption spectroscopy revealed ultrafast interfacial charge transfer from WO3 to g-C3N4. The optimized heterostructure exhibited considerably photocatalytic activity, achieving a 2571.6 μmol g−1 h−1 H2O2 production rate, representing 2.8- and 63.5-fold improvements over g-C3N4 and WO3, respectively. Electron paramagnetic resonance and in situ diffuse reflectance infrared Fourier-transform spectroscopy were used to elucidate the oxygen reduction reaction mechanism, indicating that ethanol undergoes sequential oxidation, whereas photogenerated electrons reduce O2 to produce H2O2 through a sequential single-electron process. This study offers significant mechanistic insights into the carrier dynamics within 2D S-scheme heterojunctions and presents a scalable and efficient route for green H2O2 synthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 333-345"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214577","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

Unraveling structure-activity relationships in 2-D covalent organic frameworks for photocatalysis: From molecular engineering to high-performance optimization 揭示二维共价有机框架光催化的构效关系：从分子工程到高性能优化

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)65021-8

Jiaying Liu , Yu Fang

{"title":"Unraveling structure-activity relationships in 2-D covalent organic frameworks for photocatalysis: From molecular engineering to high-performance optimization","authors":"Jiaying Liu , Yu Fang","doi":"10.1016/S1872-2067(26)65021-8","DOIUrl":"10.1016/S1872-2067(26)65021-8","url":null,"abstract":"<div><div>Faced with national fossil energy depletion and worsening environmental pollution, the shift to renewable energy is urgent. Solar energy, as a green and eco-friendly option, is converted into storable secondary energy to achieve carbon neutrality. Photocatalysts are key for this solar-to-secondary energy conversion, and two-dimensional covalent organic frameworks (2-D COFs) are highly promising candidates due to their large specific surface area, excellent stability, and flexible structural design. This paper comprehensively reviews the structural design of 2-D COFs, photocatalytic mechanisms, and the structure-function relationship. It also explores their applications in six fields: carbon dioxide reduction for carbon mitigation, uranium extraction from seawater for resource security, hydrogen peroxide synthesis as an eco-friendly alternative, organic transformation with high selectivity, and pollutant degradation for environmental improvement and hydrogen synthesis as a renewable energy. However, 2-D COFs face challenges in the photocatalytic field, including a limited light absorption range and relatively low charge separation efficiency. These issues hinder their full-scale application and performance optimization. Despite these obstacles, this study provides key insights and future directions for advancing 2-D COFs, aiming to inspire further research to overcome current limitations and unlock their full potential.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 47-87"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214583","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

Metal-free fluorinated carbon nitride with piezo-boosted hydrogen-bonding networks enable 100% CO selectivity in CO2 reduction 无金属氟化碳氮与压电增强氢键网络实现100% CO选择性CO2减少

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)65035-8

Xingchen He , Junhui Shao , Najun Li , Dongyun Chen , Hua Li , Qingfeng Xu , Haozhi Wang , Jianmei Lu

{"title":"Metal-free fluorinated carbon nitride with piezo-boosted hydrogen-bonding networks enable 100% CO selectivity in CO2 reduction","authors":"Xingchen He , Junhui Shao , Najun Li , Dongyun Chen , Hua Li , Qingfeng Xu , Haozhi Wang , Jianmei Lu","doi":"10.1016/S1872-2067(26)65035-8","DOIUrl":"10.1016/S1872-2067(26)65035-8","url":null,"abstract":"<div><div>The efficient conversion of CO2 into industrial fuels via piezocatalysis is a compelling solution to carbon emissions but often suffers from low activity and poor selectivity. While many piezocatalysts contain metals, the metal-free and low-cost graphitic carbon nitride (g-C3N4) is a promising alternative. However, its modest piezoelectric response and intrinsically low surface activity are unfavorable for efficient CO2 activation. Here, we demonstrate that halogen doping transforms its catalytic capability by creating highly active hybridized p-states near the Fermi level. Fluorine doping introduces F 2p orbitals that hybridize with C 2p states, forming a new, higher-energy valence band maximum. This modification simultaneously creates electronically potent sites for CO2 activation and enhances the driving force for charge separation. The resulting F-C3N4 converts CO2 exclusively to CO with 100% selectivity and a high production rate of 201.7 µmol g–1 h–1 under ultrasonic vibration without sacrificial agents. Mechanistic investigations reveal macroscopic piezoelectric polarization synergizes with a fluorine-induced local field to drive directional charge separation. Critically, reconstructed interfacial hydrogen-bond networks facilitate CO2 adsorption and activation, significantly lowering the energy barrier for *COOH formation. This dynamic coupling provides a new paradigm for designing high-efficiency CO2 reduction systems.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 130-142"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214510","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

Relationship between palladium nuclearity and catalytic activity and selectivity in acetylene semi-hydrogenation 钯核与乙炔半加氢催化活性和选择性的关系

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)64982-0

Polina Lavrik , Jurjen Cazemier , Mohamed N. Hedhili , Sudheesh K. Veeranmaril , Abdallah Nassereddine , Antonio Aguilar-Tapia , Marina Chernova , Jean-Louis Hazemann , Alla Dikhtiarenko , Javier Ruiz-Martínez

{"title":"Relationship between palladium nuclearity and catalytic activity and selectivity in acetylene semi-hydrogenation","authors":"Polina Lavrik , Jurjen Cazemier , Mohamed N. Hedhili , Sudheesh K. Veeranmaril , Abdallah Nassereddine , Antonio Aguilar-Tapia , Marina Chernova , Jean-Louis Hazemann , Alla Dikhtiarenko , Javier Ruiz-Martínez","doi":"10.1016/S1872-2067(26)64982-0","DOIUrl":"10.1016/S1872-2067(26)64982-0","url":null,"abstract":"<div><div>Optimizing the noble metal utilization and stability in catalysts for acetylene semi-hydrogenation reaction while maintaining high activity and ethylene selectivity is crucial for catalyst implementation on the industrial scale. Here we tune the reduction temperature of a single-atom Pd catalyst supported on N-doped carbon to regulate the populations of Pd species and quantify their contributions to acetylene semi-hydrogenation. X-ray absorption near-edge structure linear-combination fitting and extended X-ray absorption fine structure (EXAFS) wavelet transform analysis, complemented by in-situ EXAFS under reaction conditions, resolves the evolution from isolated Pd atoms (Pd1) to 2–3 atom ensembles (Pd2/3), clusters, and nanoparticles. Reduction at 200 °C generates around 9% Pd2/3 within a Pd1 population. Kinetic deconvolution at low conversion shows that Pd2/3 are 10 times more active than Pd1 while maintaining high ethylene selectivity and low ethane formation; in-situ EXAFS confirms the stability of these ensembles. Increasing the reduction temperature to 400 °C eliminates Pd2/3 in favor of Pd clusters whose per-site turnover frequency is around 25–30 times higher than that of Pd1 but with a slight decrease in ethylene selectivity. After reduction at 600 °C, the catalyst contains 34 ± 6% Pd nanoparticles and 17 ± 6% clusters, delivering high conversion yet reducing ethylene selectivity to ~55% and increasing ethane production, consistent with over-hydrogenation on larger Pd entities. These results establish a quantitative link between Pd nuclearity and per-site kinetics.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 384-393"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214576","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

Anchoring single/dual metal centers on carbon nitride: Sustainable routes for greenhouse gas conversion and organic photosynthesis 氮化碳锚定单/双金属中心：温室气体转化和有机光合作用的可持续路线

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)65008-5

Qing Lan , Su-Juan Jin , Ying-Ying Jiao , Zhi-Ming Zhang

{"title":"Anchoring single/dual metal centers on carbon nitride: Sustainable routes for greenhouse gas conversion and organic photosynthesis","authors":"Qing Lan , Su-Juan Jin , Ying-Ying Jiao , Zhi-Ming Zhang","doi":"10.1016/S1872-2067(26)65008-5","DOIUrl":"10.1016/S1872-2067(26)65008-5","url":null,"abstract":"<div><div>Single-atom and dual-atom catalysts (SACs/DACs) have attracted significant interest owing to their maximized atom utilization efficiency and distinctive synergistic properties. Nevertheless, the fabrication of highly efficient and stable SACs/DACs continues to present considerable challenges, largely due to elevated surface energy and the complexity of achieving precise coordination environments and spatial distribution of metallic sites. Effective regulation of chemical bonding between metal centers and supporting matrices is crucial to suppress aggregation tendencies. Carbon nitride (g-C3N4) has gained prominence as a robust scaffold for immobilizing SACs and DACs, attributed to its well-defined electronic configuration, notable chemical stability, and customizable surface characteristics. A dynamic electronic interplay is observed: metal species tailor the electronic properties of g-C3N4, while the support reciprocally modulates the catalytic behavior of metal active sites. This review comprehensively outlines recent progress in g-C3N4-based SACs and DACs, with focused discussion on synthetic methodologies, reaction mechanisms, and applications in greenhouse gas transformation and photosynthetic organic synthesis. Furthermore, the article emphasizes emerging trends in advanced characterization, precision synthesis, and the elucidation of bidirectional metal-support interactions, offering insightful directions for subsequent research in the field.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 13-33"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214581","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

Mn-Zn-O active phase promoted Ni-Co nanometal exsolved from MgO-based oxide for photothermal dry reforming of methane Mn-Zn-O活性相促进mgo基氧化物中Ni-Co纳米金属的析出，用于甲烷光热干重整

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)65002-4

Xiaofeng Yan , Yuxuan Meng , Yuefan Tuo , Yao Xue , Qianrui Yang , Zhengkun Luo , Yilong Yan , Meng Lin , Yufei Zhao , Xianguang Meng

{"title":"Mn-Zn-O active phase promoted Ni-Co nanometal exsolved from MgO-based oxide for photothermal dry reforming of methane","authors":"Xiaofeng Yan , Yuxuan Meng , Yuefan Tuo , Yao Xue , Qianrui Yang , Zhengkun Luo , Yilong Yan , Meng Lin , Yufei Zhao , Xianguang Meng","doi":"10.1016/S1872-2067(26)65002-4","DOIUrl":"10.1016/S1872-2067(26)65002-4","url":null,"abstract":"<div><div>Multicomponent synergistic catalysis offers a promising strategy to address the severe coking in dry reforming of methane (DRM). In this study, a multicomponent Ni0.05Mn0.05Co0.05Zn0.05Mg0.8O catalyst was developed, with Zn stabilized MnO (Mn-Zn-O active phase) promotes the DRM performance of exsolved NiCo nanometals from MgO-based oxide. Zn doping improves MnO dispersion and enrichment on MgO support during reduction by forming Mn-Zn-O active phase, in which Mn serves as a redox-active promoter to enhance activation and dissociation of CH4 and CO2. The reduction of Mn to a lower valence state can facilitate CO2 adsorption and dissociation on the surface of catalysts, which also enhanced oxygen mobility to promote CH4 activation and coke removal. The optimized Ni0.05Mn0.05Co0.05Zn0.05Mg0.8O catalyst demonstrates exceptional stability in thermal DRM at 800 °C for 100 h. And in photothermal DRM, the catalyst also achieves outstanding activity under high gas flow rates with well-designed three-dimensional porosity catalytic reactor.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 298-309"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214515","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 Cu-incorporated NASICON catalyst executing one-step conversion of methanol and acetic acid to acrylic acid and its esters Cu-incorporated NASICON催化剂，甲醇和乙酸一步转化为丙烯酸及其酯

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)65014-0

Jiahao Wang , Qiliang Gao , Chao Li , Xiujuan Gao , Jian Gong , Faen Song , Junfeng Zhang , Yizhuo Han , Qingde Zhang

{"title":"A Cu-incorporated NASICON catalyst executing one-step conversion of methanol and acetic acid to acrylic acid and its esters","authors":"Jiahao Wang , Qiliang Gao , Chao Li , Xiujuan Gao , Jian Gong , Faen Song , Junfeng Zhang , Yizhuo Han , Qingde Zhang","doi":"10.1016/S1872-2067(26)65014-0","DOIUrl":"10.1016/S1872-2067(26)65014-0","url":null,"abstract":"<div><div>Direct synthesis of acrylic acid (AA) from methanol and acetic acid is promising for the high-value utilization of coal-based chemicals. However, this direct synthesis faces challenges due to limited catalyst functionality or insufficient synergistic effects among multiple active sites. Herein, we constructed a series of bifunctional catalysts (CuO-NSCs) by incorporating Cu into NASICON material for direct synthesis of AA. A total selectivity of 96.0% to AA, methyl acrylate (MA), and methyl acetate was achieved over a 2.5 wt% CuO-NSC catalyst, with the 56.3% selectivity of AA+MA, approximately 23% higher than the one ever reported (33%). Our research revealed that NASICON substrate promoted the formation of more Cu+ species, which are crucial redox active sites for methanol dehydrogenation into formaldehyde; furthermore, the appropriate introduction of Cu somewhat regulated surficial acid-base properties, specifically increasing the density of medium-strength acidic and basic sites that are essential for the aldolization of acetic acid and formaldehyde. Apparently, the superior activity of the catalyst was attributed to good synergistic effects between the redox sites and acid-base sites.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 356-370"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214579","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

Turning methanation into chain growth: Na-induced mechanistic bifurcation on Co-ZrOx catalyst 甲烷化转化为链式生长：Co-ZrOx催化剂上na诱导的机制分叉

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)65033-4

Syeda Sidra Bibi , Sheraz Ahmed , Heuntae Jo , Jaehoon Kim

{"title":"Turning methanation into chain growth: Na-induced mechanistic bifurcation on Co-ZrOx catalyst","authors":"Syeda Sidra Bibi , Sheraz Ahmed , Heuntae Jo , Jaehoon Kim","doi":"10.1016/S1872-2067(26)65033-4","DOIUrl":"10.1016/S1872-2067(26)65033-4","url":null,"abstract":"<div><div>Direct hydrogenation of CO2 to long-chain hydrocarbons represents a promising route for carbon-neutral fuel production, yet achieving high selectivity and catalyst stability remains a formidable challenge. In this study, we systematically investigate the promotional effect of alkali metals (Li, Na, K) on cobalt-zirconia catalysts, revealing that the nature of the alkali promoter governs both redox stability and product distribution. While unpromoted and K-promoted catalysts undergo extensive surface reoxidation during CO2 hydrogenation, suppressing C–C coupling and favoring methane formation, the Na-promoted catalyst preserves the metallic Co0 phase and achieves exceptional C5+ hydrocarbon selectivity (39.4%) and yield (22.4%) under industrially relevant conditions. Mechanistic investigations reveal that Na uniquely facilitates the formation of hydroxyl and formyl intermediates conducive to C–C bond formation, while avoiding carbonate passivation observed in the Li-promoted catalyst. This work highlights a previously unrecognized role of Na in simultaneously stabilizing active sites and directing reaction pathways, offering a rational strategy for designing robust, selective cobalt-based catalysts for CO2 conversion to liquid hydrocarbons that can be used as sustainable transportation fuel.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 394-411"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214580","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

Unraveling the superiority of Ni1-MoS2 single-atom catalyst in CO2 hydrogenation to methanol: A DFT combined microkinetic study 揭示Ni1-MoS2单原子催化剂在CO2加氢制甲醇中的优越性：DFT联合微动力学研究

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)65027-9

Lanlan Chen , Li Sheng , Yanan Zhou , Qiquan Luo , Zhenyu Li , Wenhua Zhang , Jinlong Yang

{"title":"Unraveling the superiority of Ni1-MoS2 single-atom catalyst in CO2 hydrogenation to methanol: A DFT combined microkinetic study","authors":"Lanlan Chen , Li Sheng , Yanan Zhou , Qiquan Luo , Zhenyu Li , Wenhua Zhang , Jinlong Yang","doi":"10.1016/S1872-2067(26)65027-9","DOIUrl":"10.1016/S1872-2067(26)65027-9","url":null,"abstract":"<div><div>Converting CO2 to methanol presents a crucial pathway for achieving carbon neutrality, yet designing highly active and selective nano catalysts remain challenging. In this work, we report a combined density functional theory and microkinetic study screening 26 transition metal single atoms (Sc-Zn, Y-Cd, Ta-Au) atomically dispersed in MoS2 nanosheet (M1-MoS2) for CO2 hydrogenation to methanol. Among these, Ni1-MoS2 was identified as a promising candidate, exhibiting excellent stability and hydrogen dissociation capability. The reaction proceeds through a dissociative hydrogenation mechanism via key intermediates including *COOH, *C(OH)2, *CH(OH)2, *CHOH, and *CH2OH. Microkinetic simulations reveal that Ni1-MoS2 significantly outperforms the experimentally validated Pt1-MoS2, demonstrating a 26.76-fold enhancement in formation rate and high selectivity under industrial relevant conditions (210 °C, 8 bar CO2, 24 bar H2). This work not only highlights Ni1-MoS2 as a highly efficient and cost-effective catalyst but also provides a mechanistic and kinetic framework for accelerating the design of single-atom catalysts for CO2 conversion.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 143-152"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214511","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

Surface anions-mediated dynamic interfacial free water enriched microenvironment on RuO2 for efficient acidic oxygen evolution 表面阴离子介导的动态界面自由水富集RuO2微环境对酸性氧的高效析出

IF 17.7 1区化学

Chinese Journal of Catalysis Pub Date : 2026-06-01 Epub Date: 2026-06-11 DOI: 10.1016/S1872-2067(26)64993-5

Liqing Wu , Wenxia Huang , Bingbing Zhao , Ping Cai , Wei Luo

{"title":"Surface anions-mediated dynamic interfacial free water enriched microenvironment on RuO2 for efficient acidic oxygen evolution","authors":"Liqing Wu , Wenxia Huang , Bingbing Zhao , Ping Cai , Wei Luo","doi":"10.1016/S1872-2067(26)64993-5","DOIUrl":"10.1016/S1872-2067(26)64993-5","url":null,"abstract":"<div><div>Recent studies have revealed that the slow kinetics of active free water molecule replenishment on the surface of catalyst can be the potential cause responsible for the sluggish reaction kinetics of oxygen evolution reaction (OER) under acidic electrolyte. However, engineering the dynamic interfacial water structure to form the free water enriched microenvironment has rarely been implemented due to the relatively inherent inert catalyst surface. Herein, we demonstrate that surface modification of ruthenium dioxide (RuO2) with PO43– anions (RuP0.4Ox) can effectively regulate the free water enriched microenvironment and significantly enhance the acidic OER performance. Experimental results including operando attenuated total reflectance surface-enhanced infrared absorption spectroscopy reveal that the introduction of PO43– species can manipulate the interfacial water structure, resulting in a free-H2O-enriched interfacial environment, which is conducive to the continuous supply of reactants. Moreover, theoretical studies indicate that the surface modified PO43– could facilitate proton transfer to the oxygen sites of the PO43– group, enabling a PO43–-assisted adsorption evolution mechanism with enhanced reaction kinetics. Consequently, the obtained RuP0.4Ox catalyst, featuring a Ru-O-P local environment and modified by surface PO43– anions, displays a low overpotential of 200 mV at 10 mA cm–2 and operates stably for 500 h during the acidic OER process.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"85 ","pages":"Pages 237-246"},"PeriodicalIF":17.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148214572","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