Chinese Journal of Catalysis最新文献_第3页

Multi-intermolecular forces strengthen interfacial carrier mobility in poly (barbituric acid) all-organic heterojunction systems for efficient solar-to-hydrogen conversion 多分子间力增强了聚巴比妥酸全有机异质结系统的界面载流子迁移率，实现了高效的太阳能-氢转化

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 DOI: 10.1016/S1872-2067(25)64845-5

Zhe Zhang , Guixu Pan , Wei Zhu , Keyu Zhang , Guijie Liang , Shihan Wang , Ning Wang , Yan Xing , Yunfeng Li

The development of high-performance all-organic heterojunction photocatalytic systems and the elucidation of their charge carrier excitation and interface migration dynamics have attracted significant research interest. Herein, poly (barbituric acid)/g-C₃N₄ (PBA/UCN) all-organic heterojunctions were prepared by exploiting multiple intermolecular interactions to induce fast interface charge-carrier transfer with a lifetime of approximately 5.05 ps, as was directly verified by in-situ Kelvin probe force microscopy and in-situ irradiation X-ray photoelectron spectroscopy. Moreover, the dynamics and lifetimes of charge carriers were studied by fitting the decay curves of excited-state absorption signals at 600 nm and ground-state bleaching signals at 495 nm obtained by femtosecond transient absorption spectroscopy to further reveal the diffusion, relaxation, and transfer processes of PBA/UCN. The as-prepared PBA/UCN all-organic molecular heterojunction with optimal redox ability exhibits an excellent H₂ evolution rate of 12.55 mmol h^–1 g^–1 and an apparent quantum efficiency of 17.12% at 420 ± 15 nm. In particular, we demonstrate that PBA, which is a promising oxidizing organic semiconductor, can be coupled with various reducing organic photocatalytic materials such as poly(triazine imide), poly(heptazine imide), perylene-3,4,9,10- tetracarboxylic acid, and covalent triazine-based frameworks to obtain a series of efficient all-organic heterojunction photocatalysts.

高性能全有机异质结光催化体系的开发及其载流子激发和界面迁移动力学的研究引起了人们的极大兴趣。通过原位开尔文探针力显微镜和原位辐照x射线光电子能谱直接验证了聚巴比妥酸/g-C3N4 （PBA/UCN）全有机异质结的制备，并利用多种分子间相互作用诱导界面电荷-载流子快速转移，其寿命约为5.05 ps。此外，通过拟合飞秒瞬态吸收光谱获得的600 nm激发态吸收信号和495 nm基态漂白信号的衰减曲线，研究了载流子的动力学和寿命，进一步揭示了PBA/UCN的扩散、弛豫和转移过程。制备的PBA/UCN全有机分子异质结具有最佳的氧化还原能力，在420±15 nm处，H2的析出速率为12.55 mmol h-1 g-1，表观量子效率为17.12%。特别是，我们证明了PBA是一种很有前途的氧化性有机半导体，它可以与各种还原性有机光催化材料如聚（三嗪亚胺）、聚（七嗪亚胺）、苝-3,4,9,10-四羧酸和共价三嗪基框架偶联，得到一系列高效的全有机异质结光催化剂。

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引用次数: 0

Cu-Mo synergistic doping of metal-organic framework double-shelled hollow nanospheres: Surface reconstruction activates adsorbate evolution and lattice oxygen mechanisms 金属-有机骨架双壳空心纳米球的Cu-Mo协同掺杂：表面重构激活吸附质演化和晶格氧机制

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 DOI: 10.1016/S1872-2067(25)64862-5

Yu Tang , Yang Chen , Kerun Chen , Edmund Qi , Xiaoyang Liu , Haiyan Lu , Yu Gao

In order to attain high catalytic activity and long-term stability in the oxygen evolution reaction (OER), it is essential to design catalysts with hollow structures that integrate both the adsorbate evolution mechanism (AEM) and the lattice oxygen mechanism (LOM). Based on the above issues, we developed a novel templating method and, for the first time, synthesized double-shelled hollow nanospheres of ZIF-67. Utilizing the inherent hollow structure and chemical activity of ZIF-67, and through Cu-Mo co-doping, we prepared a CuCo₂S₄/MoS₂ OER catalyst with dual mechanisms. The Jahn-Teller effect of copper activates lattice oxygen, facilitating LOM in OER. The cooperative interaction between copper and molybdenum atoms induces surface reconstruction in the catalyst, accelerates the deprotonation step in LOM, and aids in the formation of *OOH in AEM, thus reducing energy barriers and optimizing the adsorption of reaction intermediates. The addition of molybdenum further boosts catalytic performance by enhancing both mechanisms, owing to the spatial disparity between Cu and Mo atoms. Due to the compatibility of the dual mechanisms, the catalyst demonstrates outstanding electrochemical performance in alkaline media (320 mV at 100 mA cm⁻²) and maintains a stable catalytic current in a commercial water-splitting device (500 mA cm⁻² for 300 h). This study presents an innovative strategy for designing oxygen evolution reaction catalysts that integrate both AEM and LOM mechanisms. Considering the widespread applications of ZIF-67 in electrocatalysis and electrochemical energy storage, CuCo-G@ZIF-67 not only serves as a versatile precursor for the synthesis of various catalysts but also paves the way for the development of novel transition metal catalysts and multi-shell energy storage materials.

为了在析氧反应（OER）中获得高的催化活性和长期的稳定性，必须设计同时具有吸附质析氧机制（AEM）和晶格析氧机制（LOM）的中空结构催化剂。基于以上问题，我们开发了一种新的模板化方法，首次合成了ZIF-67双壳中空纳米球。利用ZIF-67固有的空心结构和化学活性，通过Cu-Mo共掺杂，制备了具有双机理的CuCo2S4/MoS2 OER催化剂。铜的Jahn-Teller效应激活了晶格氧，促进了OER中的LOM。铜和钼原子之间的协同相互作用在催化剂中诱导了表面重构，加速了LOM中的去质子化步骤，并有助于AEM中*OOH的形成，从而降低了能垒，优化了反应中间体的吸附。由于Cu和Mo原子之间的空间差异，钼的加入通过增强这两种机制进一步提高了催化性能。由于双机制的相容性，该催化剂在碱性介质（100 mA cm−2,320 mV）中表现出优异的电化学性能，并在商用水分解装置（500 mA cm−2,300 h）中保持稳定的催化电流。本研究提出了一种结合AEM和LOM机制的析氧反应催化剂的创新设计策略。考虑到ZIF-67在电催化和电化学储能方面的广泛应用，CuCo-G@ZIF-67不仅是合成各种催化剂的多功能前驱体，而且为新型过渡金属催化剂和多壳储能材料的发展铺平了道路。

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引用次数: 0

Bipyridine-integrated bisoxazole-based donor-acceptor covalent organic framework for enhanced photocatalytic H2O2 synthesis 基于联吡啶整合双恶唑的供受体共价有机框架用于增强光催化H2O2合成

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 DOI: 10.1016/S1872-2067(25)64864-9

Jiaping Lu , Chao Lin , Chao Li , Hongjie Shi , Nengyi Liu , Wandong Xing , Sibo Wang , Guigang Zhang , Teng-Teng Chen , Xiong Chen

The deliberate integration and precise arrangement of electron donor (D) and acceptor (A) moieties within the crystalline lattices of covalent organic frameworks (COFs) represent a sophisticated strategy to optimize charge separation and electron transfer processes, thereby enhancing photocatalytic efficiency. Herein, we report the rational design and synthesis of two novel bisoxazole-based D-A type COFs, designated as Bpy-COF and Bph-COF. These frameworks incorporate identical acceptor units but are distinguished by their unique donor motifs, enabling a comparative evaluation of their structural and functional properties. The results reveal that Bpy-COF, which incorporates bipyridyl (Bpy) donor moieties, exhibits superior photocatalytic H₂O₂ production performance compared to Bph-COF, potentially related to its broader light response range and increased availability of reactive sites. Furthermore, the coplanar and conjugated nature of the Bpy groups facilitates efficient charge separation and migration, thereby accelerating the two-electron oxygen reduction reaction critical to H₂O₂ synthesis. This study affirms the effectiveness of manipulating the structural components of COF photocatalysts, propelling new insights for the design and synthesis of high-performance catalysts.

在共价有机框架（COFs）的晶格中，电子给体(D)和受体(A)部分的精心整合和精确排列代表了优化电荷分离和电子转移过程的复杂策略，从而提高光催化效率。本文报道了两种新型双恶唑类D-A型coof的合理设计和合成，分别命名为Bpy-COF和Bph-COF。这些框架包含相同的受体单元，但以其独特的供体基序进行区分，从而可以对其结构和功能特性进行比较评估。结果表明，与Bph-COF相比，含有联吡啶基（Bpy）供体的Bpy- cof表现出更好的光催化产H2O2性能，这可能与Bph-COF更宽的光响应范围和更高的反应位点可用性有关。此外，Bpy基团的共面和共轭性质有利于有效的电荷分离和迁移，从而加速了对H2O2合成至关重要的双电子氧还原反应。该研究证实了操纵COF光催化剂结构组分的有效性，为高性能催化剂的设计和合成提供了新的见解。

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引用次数: 0

Charge-mediated cyclohexanone enrichment and intermediate stabilization at MoNi4/MoO2 heterostructures enable paired cyclohexanone electrooxidation-hydrogen production at ampere-level current 电荷介导的环己酮富集和在MoNi4/MoO2异质结构上的中间稳定使得配对环己酮在安培电流下电氧化制氢成为可能

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 DOI: 10.1016/S1872-2067(25)64858-3

Rui Yang , Zimin Han , Yin Gao , Guoqing Feng , Huaizhi Liu , Yiyin Huang , Zhongkai Wang , Yaobing Wang

Electrocatalytic oxidation of cyclohexanone (KOR) to adipic acid provides a sustainable and value-added pathway for coupled hydrogen evolution (HER). However, the weak adsorption of the reactants and intermediates leads to poor reaction kinetics and product yield. Herein, we synthesized MoNi₄/MoO₂ heterostructures via phase conversion to engineer a large work function difference that optimizes the Ni electronic structure. This design enhances cyclohexanone adsorption and regulates intermediates, achieving 85% Faradaic efficiency for production of adipic acid and a 2 mmol h^–1 cm^–2 production rate, along with an ampere-level current. In a membrane electrode assembly electrolyzer for KOR-assisted HER, this catalyst displays 1 A current with 12.1 mol adipic acid production and 3.34 L H₂ generation over 8 h, maintaining stability for 56 h at 3 A. Optimized Ni electronic structure achieved through heterojunction-induced charge redistribution strengthens cyclohexanone adsorption and lowers the energy barriers for key intermediates (C₆H₁₀O₂* and C₆H₁₀O₃*), boosting oxidation activity. This study presents a novel heterojunction engineering strategy that synergistically enhances reactant adsorption and optimizes intermediate reaction kinetics, offering a tailored approach for efficient catalytic systems.

电催化氧化环己酮（KOR）制己二酸为耦合析氢（HER）提供了一条可持续和增值的途径。然而，对反应物和中间体的弱吸附导致反应动力学和产物收率较差。在此，我们通过相变合成了MoNi4/MoO2异质结构，设计了一个大的功函数差，优化了Ni电子结构。该设计增强了环己酮的吸附并调节了中间体，使己二酸的法拉第效率达到85%，产率为2 mmol h-1 cm-2，电流为安培级。在kor辅助HER的膜电极组装电解槽中，该催化剂在1 a电流下产生12.1 mol己二酸，在8 h内产生3.34 L H2，在3 a电流下保持稳定56 h。通过异质结诱导电荷重分配优化的Ni电子结构增强了环己酮的吸附，降低了关键中间体（C6H10O2*和C6H10O3*）的能垒，提高了氧化活性。本研究提出了一种新的异质结工程策略，可以协同增强反应物吸附并优化中间反应动力学，为高效催化系统提供量身定制的方法。

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引用次数: 0

Towards highly efficient selective hydrogenation: The role of single-atom catalysts 迈向高效选择性加氢：单原子催化剂的作用

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 DOI: 10.1016/S1872-2067(25)64906-0

Peikun Li , Jinghui Lyu , Yiyong Zhao , Han Wu , Xianghao Zhang , Qiannan Lu , Yizhi Xiang , Blaž Likozar , Matej Huš , Adriana Zaleska-Medynska , Xiaonian Li

Selective hydrogenation is crucial in various chemical processes and environmental applications, where precise control of reactivity and selectivity is essential for the efficient production of high-purity products. Single-atom catalysts (SACs), with atomically dispersed metal sites, could bridge homogeneous and heterogeneous catalysis and have emerged as a transformative platform for highly efficient selective hydrogenation with minimal use of critical raw materials as catalysts. This review explores the latest advancements in this cutting-edge area. Specifically, we analyze the structure-activity relationships, such as catalytic properties and mechanisms that determine the reactivity and selectivity of such catalytic systems. Furthermore, we discuss challenges, including stability, synthesis scalability, coordination environment tuning, atomistic modeling, and mechanistic insights, while identifying research opportunities for optimizing SACs performance. If these challenges are addressed, SACs hold the potential to revolutionize selective hydrogenation processes, offering sustainable and highly efficient catalytic solutions for industrial applications.

选择性加氢在各种化学过程和环境应用中至关重要，其中精确控制反应性和选择性对于高效生产高纯度产品至关重要。单原子催化剂（SACs）具有原子分散的金属位点，可以架起均相和多相催化的桥梁，并且已经成为一种变革性的平台，可以在最少使用关键原料作为催化剂的情况下实现高效选择性氢化。本文综述了这一前沿领域的最新进展。具体来说，我们分析了结构-活性关系，如催化性质和机制，决定了这种催化系统的反应性和选择性。此外，我们还讨论了挑战，包括稳定性、综合可扩展性、协调环境调优、原子建模和机制见解，同时确定了优化sac性能的研究机会。如果这些挑战得到解决，SACs有可能彻底改变选择性加氢过程，为工业应用提供可持续和高效的催化解决方案。

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引用次数: 0

Advances in metal oxide catalysts for efficient VOCs oxidation: Synthesis strategy and catalytic mechanism 金属氧化物高效氧化VOCs催化剂的研究进展：合成策略及催化机理

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 DOI: 10.1016/S1872-2067(25)64891-1

Fan Dang , Chunli Ai , Chi Ma , Zeyu Jiang , Jicheng Liu , Mingjiao Tian , Mingzhuo Zhang , Chi He

The severe hazard of volatile organic compounds (VOCs) makes their decomposition technology a key topic research. Catalytic oxidation is an efficient and environmentally friendly strategy for removing VOCs. The metal oxide catalysts dominate VOCs oxidation reactions, owing to their cost-effectiveness, robust redox properties, tunable crystal structures, and excellent operational stability. Thus, designing high-performance metal oxide catalysts is important. This review systematically summarized the recent advances in constructing highly efficient active metal oxides, with emphasis on representative preparation method, the structure performance relationship, and the reaction mechanism of different types VOCs. Finally, the remaining challenges for creating metal oxide catalysts in practical applications are discussed.

挥发性有机物（VOCs）的严重危害使其分解技术成为研究的重点课题。催化氧化是一种高效、环保的去除挥发性有机化合物的方法。金属氧化物催化剂因其成本效益、强大的氧化还原性能、可调谐的晶体结构和优异的操作稳定性而在VOCs氧化反应中占据主导地位。因此，设计高性能的金属氧化物催化剂是非常重要的。本文系统综述了近年来构建高效活性金属氧化物的研究进展，重点介绍了具有代表性的制备方法、不同类型VOCs的结构性能关系以及反应机理。最后，讨论了在实际应用中制备金属氧化物催化剂所面临的挑战。

引用次数: 0

Self-assembling 3D/2D ZnIn2S4/CN-NH4 to construct S-scheme heterojunctions for the efficient production of H2O2 in pure water 自组装3D/2D ZnIn2S4/CN-NH4构建s型异质结，用于纯水中H2O2的高效生成

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 DOI: 10.1016/S1872-2067(25)64851-0

Congcong Wang , Yongkang Quan , Suili Shi , Guorong Wang , Zhiliang Jin

The photocatalytic double-electron oxygen reduction pathway has become a strategic approach for the production of hydrogen peroxide (H₂O₂). In many heterojunction systems, indium zinc sulfide (ZnIn₂S₄) has received increasing attention, but it is limited by its slow REDOX kinetics and the lack of sufficient double-electron oxygen reduction active sites. In this study, low-cost CN-NH₄ fragments were loaded onto flower-like indium zinc sulfide (ZnIn₂S₄) to construct a compact S-scheme, in order to achieve environmentally friendly hydrogen peroxide photosynthesis. The H₂O₂ yield of the ZnIn₂S₄/CN-NH₄ photocatalyst was 2031 µmol g^–1 h^–1, which was 2.84 and 21.39 times that of ZnIn₂S₄ and CN-NH₄, respectively. This is attributed to the contact between ZnIn₂S₄ and CN-NH₄, providing a fast migration channel for electrons, forming a strong internal electric field at the interface, and effectively prolonging the migration lifetime of photogenerated carriers. The introduction of CN-NH₄ enhances the absorption of oxygen by ZnIn₂S₄ and simultaneously reduces the energy barrier of its two-electron oxygen reduction reaction. This study provides a new approach for constructing S-scheme heterojunction materials that can efficiently generate H₂O₂ under solar irradiation.

光催化双电子氧还原途径已成为生产过氧化氢（H2O2）的战略途径。在许多异质结体系中，硫化铟锌（ZnIn2S4）受到越来越多的关注，但由于其氧化还原动力学缓慢和缺乏足够的双电子氧还原活性位点而受到限制。本研究将低成本的CN-NH4片段加载到花状的硫化铟锌（ZnIn2S4）上，构建紧凑的S-scheme，以实现环境友好的过氧化氢光合作用。ZnIn2S4/CN-NH4光催化剂的H2O2产率为2031µmol g-1 h-1，分别是ZnIn2S4和CN-NH4的2.84倍和21.39倍。这是由于ZnIn2S4与CN-NH4接触，为电子提供了快速迁移通道，在界面处形成强大的内部电场，有效延长了光生载流子的迁移寿命。CN-NH4的引入增强了ZnIn2S4对氧的吸收，同时降低了其双电子氧还原反应的能垒。本研究为构建能在太阳辐照下高效生成H2O2的s型异质结材料提供了新途径。

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引用次数: 0

Enhanced photocatalytic production of hydrogen and benzaldehyde over a dual-function ZnxCd1–xSy/FePS3 S-scheme heterojunction 双功能ZnxCd1-xSy /FePS3 S-scheme异质结增强光催化制氢和苯甲醛

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64830-3

Rundong Chen , Yuhang Zhang , Bingquan Xia , Xianlong Zhou , Yanzhao Zhang , Shantang Liu

Photocatalysis is deemed a green approach to sustainable energy conversion with great promise for addressing future energy challenges. However, traditional photocatalytic systems are often inhibited by rapid recombination of photogenerated electron-hole pairs and low light-harvesting efficiency. To overcome these challenges, an S-scheme heterojunction integrating Zn_xCd_1–xS_y (ZCS) nanocrystals with FePS₃ (FPS) nanosheets was designed to facilitate both photocatalytic hydrogen evolution and the conversion of benzyl alcohol to benzaldehyde (BAD). The obtained ZCS/FPS-15 (ZCSF-15) heterostructure exhibits remarkable visible-light-harvesting enhancement and charge separation efficiency, delivering a hydrogen evolution rate of 73.06 mmol g⁻¹ h⁻¹ and a BAD production rate of 46.68 mmol g⁻¹ h⁻¹, corresponding to 22.34- and 53.65-fold performance enhancements, respectively, compared with that of bare ZCS. To reveal the charge transfer dynamics and clarify the reaction mechanisms, in-situ diffuse-reflectance Fourier-transform infrared spectroscopy was used to identify key oxidation intermediates, coupled with interfacial charge transfer dynamics probed using in-situ X-ray photoelectron spectroscopy and atomic force microscopy-Kelvin probe force microscopy. This work establishes a dual-function heterojunction model, offering valuable insights into how to design S-scheme heterojunctions for simultaneous green fuel generation and selective organic synthesis.

光催化被认为是一种绿色的可持续能源转换方法，对解决未来的能源挑战有很大的希望。然而，传统的光催化系统经常受到光生成的电子-空穴对快速重组和低光收集效率的抑制。为了克服这些挑战，设计了一种将ZnxCd1-xSy （ZCS）纳米晶体与FePS3 （FPS）纳米片集成在一起的S-scheme异质结，以促进光催化析氢和苯甲醇转化为苯甲醛（BAD）。得到的ZCS/FPS-15 （ZCSF-15）异质结构具有显著的可见光捕获增强和电荷分离效率，析氢速率为73.06 mmol g−1 h−1，BAD生成速率为46.68 mmol g−1 h−1，性能分别比裸ZCS提高22.34倍和53.65倍。为了揭示电荷转移动力学和阐明反应机理，采用原位漫反射傅里叶变换红外光谱技术鉴定了关键的氧化中间体，并利用原位x射线光电子能谱和原子力显微镜-开尔文探针力显微镜探测了界面电荷转移动力学。这项工作建立了一个双功能异质结模型，为如何设计s方案异质结同时用于绿色燃料生成和选择性有机合成提供了有价值的见解。

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引用次数: 0

Spin density symmetry breaking-mediated hydrogen evolution in single-atom catalysts 单原子催化剂中自旋密度对称破缺介导的析氢

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64837-6

Xin Song , Zhonghua Li , Li Sheng , Yang Liu

Symmetry-broken single-atom catalysts (SACs) are pivotal due to their asymmetric electronic environments, which enhance the activity of the hydrogen evolution reaction (HER). This study investigated how symmetry breaking in SACs affects HER performance using density functional theory (DFT) and variable selection machine learning (ML). The study revealed a nearly volcano-shaped correlation between the degree of spin density symmetry breaking (D_asym) and HER activity, with catalysts at the base of the volcano showing enhanced HER activity. Spin density symmetry breaking facilitates the enrichment of unpaired electrons on the active sites and reduces HER energy barriers, resulting in up to a 40-fold enhancement in HER performance of symmetry-broken SACs compared to symmetric SACs. The ML model accurately identified key descriptors, such as symmetry breaking and electronic transfer effects, allowing spin density symmetry breaking on M-N3C-SWCNTs to be further condensed into an effect term with a structure-property relationship. A weaker symmetry breaking effect and a stronger electron transfer enhance HER performance. ML-guided analysis highlighted a spin selection-related Volmer-Heyrovsky pathway with a dual activation mechanism involving surface atom displacement and para-activation. These findings offer critical insights into the design of advanced HER catalysts by elucidating the interplay between symmetry-breaking properties and catalytic behavior.

对称破缺单原子催化剂（SACs）由于其不对称的电子环境，提高了析氢反应（HER）的活性。本研究利用密度泛函理论（DFT）和变量选择机器学习（ML）研究了SACs中的对称性破缺如何影响HER性能。该研究揭示了自旋密度对称破缺程度（Dasym）与HER活性之间几乎呈火山状的相关性，火山底部的催化剂显示出更高的HER活性。自旋密度对称破缺促进了活性位点上未配对电子的富集，降低了she能量势垒，导致对称破缺SACs的she性能比对称SACs提高了40倍。ML模型准确地识别了关键描述符，如对称破断和电子转移效应，从而使M-N3C-SWCNTs上的自旋密度对称破断进一步浓缩为具有结构-性质关系的效应项。较弱的对称破缺效应和较强的电子转移增强了HER的性能。机器学习引导的分析强调了与自旋选择相关的Volmer-Heyrovsky途径，该途径具有双重激活机制，包括表面原子位移和副激活。这些发现通过阐明对称破坏性质和催化行为之间的相互作用，为高级HER催化剂的设计提供了重要的见解。

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引用次数: 0

Tuning radical generation rate for efficient CH4 photooxidation to CH3OH over AgPd alloy and Co3O4 cascade active sites 调节AgPd合金和Co3O4级联活性位点上CH4光氧化生成CH3OH的自由基生成速率

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-01-01 DOI: 10.1016/S1872-2067(25)64854-6

Shuqi Liang , Zhen Xiao , Jinni Shen , Wenxin Dai , Zizhong Zhang

The direct conversion of methane into methanol under mild conditions represents a highly appealing pathway. Regulating the generation of hydroxyl radicals (•OH) is a representative method, but excessive release of •OH will inevitably lead to the over-oxidation of CH₃OH. Here, we design AgPd alloy and Co₃O₄ cascade active sites on the TiO₂ surface (AgPd-Co/TiO₂) to control the release rate of •OH to improve the selectivity of CH₃OH. By incorporating Co₃O₄ as a hole buffer and storage center, the kinetics of •OH generation at the TiO₂ interface can be effectively modulated. This confines the spatial distribution of •OH to the active sites of the AgPd alloy, thus facilitating the directional combination of •CH₃ and •OH. The optimal AgPd-Co/TiO₂ photocatalyst demonstrates outstanding catalytic performance with the selectivity of CH₃OH reaching up to 93% in the liquid phase. AgPd-Co/TiO₂ exhibited significantly enhanced selectivity relative to reported TiO₂-based photocatalytic systems, while simultaneously achieving comparable methanol yields. This research offers valuable insights for the precise design of composite photocatalysts to achieve highly selective methane oxidation.

在温和条件下将甲烷直接转化为甲醇是一种非常有吸引力的途径。调节羟基自由基（•OH）的生成是一种有代表性的方法，但过量释放•OH必然会导致CH3OH的过度氧化。本研究通过在TiO2表面设计AgPd合金和Co3O4级联活性位点（AgPd- co /TiO2）来控制•OH的释放速率，从而提高CH3OH的选择性。通过加入Co3O4作为空穴缓冲和存储中心，可以有效地调节TiO2界面上•OH生成的动力学。这将•OH的空间分布限制在AgPd合金的活性位点，从而促进了•CH3和•OH的定向结合。优化后的AgPd-Co/TiO2光催化剂在液相中对CH3OH的选择性高达93%，表现出优异的催化性能。AgPd-Co/TiO2相对于已有报道的基于TiO2的光催化体系表现出显著增强的选择性，同时获得相当的甲醇产率。该研究为精确设计复合光催化剂以实现高选择性甲烷氧化提供了有价值的见解。

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引用次数: 0