Chinese Journal of Catalysis最新文献_第4页

Efficient photocatalytic hydrogen production by a heterojunction strategy with covalent organic frameworks loaded with non-precious-metal semiconductors 利用负载非贵金属半导体的共价有机骨架的异质结策略进行高效光催化制氢

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64904-7

Bolin Yang , Fei Jin , Zhiliang Jin

Rational energy band engineering and the exposure of catalytically active sites critically enhance the efficiency of the hydrogen evolution reaction. In this study, TAPT-TFPT-COF/Mn_0.2Cd_0.8S composite photocatalysts were prepared by wet impregnation. The energy bands of non-precious-metal sulfide nanorods and a covalent organic framework (COF) were interleaved for effective heterojunction construction, enabling a three-fold enhancement in hydrogen evolution compared to that of the pure Mn_0.2Cd_0.8S catalyst. The enhanced catalyst performance is attributed to the construction of heterojunctions and the synergistic photothermal dynamics of the flexible monomers under illumination, which facilitates localized charge carrier migration. Furthermore, the hydrogen evolution mechanism in the Mn_0.2Cd_0.8S/COF composites was elucidated through photoelectrochemical experiments, in-situ irradiation X-ray photoelectron spectroscopy, surface photovoltage measurements, and density functional theory. The loaded organic semiconductor materials were combined with non-precious-metal semiconductors to construct S-scheme heterojunctions with increased hydrophilicity, and the tight combination of Mn_0.2Cd_0.8S and COF optimized the photogenerated electron utilization efficiency.

合理的能带工程和催化活性位点的暴露对析氢反应的效率有重要的提高作用。本研究采用湿浸渍法制备了tpt - tfpt - cof /Mn0.2Cd0.8S复合光催化剂。非贵金属硫化物纳米棒和共价有机骨架（COF）的能带相互交错，有效地构建异质结，使析氢能力比纯Mn0.2Cd0.8S催化剂提高了三倍。催化剂性能的增强是由于异质结的构建和柔性单体在光照下的协同光热动力学，促进了局部载流子的迁移。此外，通过光电化学实验、原位辐照x射线光电子能谱、表面光电压测量和密度泛函理论，阐明了Mn0.2Cd0.8S/COF复合材料的析氢机理。将负载的有机半导体材料与非贵金属半导体材料结合，构建了亲水性增强的S-scheme异质结，Mn0.2Cd0.8S与COF的紧密结合优化了光电子利用效率。

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引用次数: 0

Tail group structure effect of ligand-protected gold nanocluster catalysts on electrochemical CO2 reduction 配体保护金纳米团簇催化剂尾基结构对电化学CO2还原的影响

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64908-4

Liting Huang , Yecheng Zhou , Yongfeng Lun, Qi Wang, Zhaobin Ding, Shuqin Song, Yi Wang

The application of thiolate-protected gold nanoclusters (NCs) for the electrochemical CO₂ reduction reaction (CO₂RR) has received widespread attentions. In this work, three types of atomically precise [Au₂₅(SR)₁₈]^‒ NCs protected by 2-phenylethanethiol (PET), 1-hexanethiol (C6T), and 1-dodecanethiol (C12T), respectively, are employed as model catalysts for CO₂RR, where the molecular configuration and length of thiolate ligands are varied. The electrochemical results demonstrate that the [Au₂₅(C12T)₁₈]^‒ NC possesses lower activity and selectivity towards CO formation than [Au₂₅(PET)₁₈]^‒ and [Au₂₅(C6T)₁₈]^‒ NCs. Owing to their identical gold kernels, the differences in electrocatalytic CO₂RR performance of these three Au₂₅ NCs can be fully attributed to their distinctions in tail group structure. Density functional theory (DFT) calculations exclude the possible effects on the electronic structures of the active sites exerted by the distinctions in tail group structure, while molecular dynamics (MD) calculations reveal that different orientation modes of tail groups in aqueous solution affect the diffusion of the reactants to active sites. Overall, this work provides a unique perspective on the structure-property relationships for ligand-protected NCs in electrocatalytic CO₂RR.

硫代酸保护金纳米团簇（NCs）在CO2电化学还原反应（CO2RR）中的应用受到了广泛关注。在本研究中，采用3种原子精密的[Au25(SR)18] - NCs分别被2-苯基乙基硫醇（PET）、1-己硫醇（C6T）和1-十二硫醇（C12T）保护，作为CO2RR的模型催化剂，其中硫酸盐配体的分子构型和长度是不同的。电化学结果表明，[Au25(C12T)18] - NC与[Au25(PET)18] -和[Au25(C6T)18] - NC相比，具有较低的CO生成活性和选择性。由于金核相同，这三种Au25 NCs电催化CO2RR性能的差异完全归因于尾基结构的差异。密度泛函理论（DFT）计算排除了尾基结构差异对活性位点电子结构的影响，而分子动力学（MD）计算揭示了水溶液中尾基的不同取向模式会影响反应物向活性位点的扩散。总的来说，这项工作为电催化CO2RR中配体保护的NCs的结构-性质关系提供了一个独特的视角。

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引用次数: 0

Insight into the role of imidazolium cations in regulating Ag electrode interface for enhancing electrochemical CO2 reduction 咪唑类阳离子调控Ag电极界面增强电化学CO2还原作用的研究

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64886-8

Diankun Song , Yunyun Wu , Jiahui Hua , Chunfeng Shao , Zhaoyang Wei , Jianji Wang , Kai Dai

Imidazolium-based ionic liquids (ILs) exhibit great potential in promoting electrochemical CO₂ reduction reaction (CO₂RR) by reducing overpotential reduction and enhancing catalytic efficiency. However, the regulatory role of ILs structure in the local physicochemical region at the electrode/electrolyte interface and in reaction kinetics remain unclear. In this study, we designed imidazolium-based ILs with tunable cation alkyl chain length and systematically revealed the dynamic interfacial regulation mechanism controlled by cation structure, based on in-situ infrared spectroscopy and molecular dynamics simulations. The commercial Ag electrodes in electrolytes with critical chain length exhibit nearly 100% Faradaic efficiency for CO production while maintaining high current density. Imidazolium cations with critical chain length effectively regulate the electric double layer at the Ag electrode/electrolyte interface: they notably balance a range of positive and negative factors, including hydrophobicity, CO₂ absorption, conductivity, viscosity, and hydrogen evolution reaction, etc. Collectively, these effects synergistically shape an optimized interfacial local physicochemical region, enhancing the rate of CO₂ catalytic reactions. This work elucidates the mechanistic framework of interfacial regulation in CO₂RR and delivers molecular design principles for engineering IL-based electrolytes toward enhanced catalytic selectivity.

咪唑基离子液体（ILs）通过减少过电位还原和提高催化效率，在促进电化学CO2还原反应（CO2RR）方面表现出巨大的潜力。然而，ILs结构在电极/电解质界面的局部物理化学区域和反应动力学中的调节作用尚不清楚。本研究基于原位红外光谱和分子动力学模拟，设计了咪唑基阳离子烷基链长度可调的il，系统揭示了阳离子结构控制的动态界面调节机制。在具有临界链长的电解液中，商用银电极在保持高电流密度的同时，具有接近100%的CO生成法拉第效率。具有临界链长的咪唑类阳离子能有效调节Ag电极/电解质界面的双电层，显著平衡了疏水性、CO2吸收、电导率、粘度、析氢反应等一系列正负因素。总的来说，这些效应协同形成了一个优化的界面局部物理化学区域，提高了CO2催化反应的速率。这项工作阐明了CO2RR中界面调节的机制框架，并为提高催化选择性的工程il基电解质提供了分子设计原则。

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引用次数: 0

Atomic-level Mn incorporation into Co3O4 for selective CO2 photoreduction in pure water under dilute CO2 atmosphere 原子水平Mn掺入Co3O4在稀CO2气氛下在纯水中选择性光还原CO2

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64861-3

Ganghua Zhou , Jie Liu , Longyun Zhang , Chuanzhou Bi , Hangmin Xu , Weiyi Jiang , Xingwang Zhu , Xin Ning , Hui Xu , Xiaozhi Wang

The photocatalytic carbon dioxide reduction represents a promising route for solar-to-chemical energy conversion, enabling the sustainable production of carbon-neutral fuels. Achieving high selectivity toward specific products remains a major challenge due to the complex multi-electron transfer pathways and competing reaction intermediates. Herein, the Mn-doped Co₃O₄ (MMC) photocatalysts are synthesized based on an “impregnation-pyrolysis” strategy using in situ synthesized Mn-doped ZIF-67 as a precursor. The MOF-templated approach enables uniform Mn incorporation into the Co₃O₄ lattice while preserving a hierarchical porous architecture, thereby enhancing active-site accessibility and modulating the electronic environment of catalyst. The introduction of guest Mn effectively suppresses the competing hydrogen evolution reaction. As a result, the optimized 2MMC catalyst shows a 12.8-fold increase in CO production over undoped Co₃O₄ and enables selective CO₂ conversion in pure water with diluted CO₂. Photoelectrochemical characterizations reveal that guest Mn doping accelerates charge separation dynamics. In-situ irradiated X-ray photoelectron spectroscopy, in-situ Fourier transformed infrared spectra, and theoretical calculations unveil a Mn-mediated pathway that selectively promotes the formation of *CO₂ and *CO intermediates. This work provides new atomic-level insights into the selective photocatalytic conversion of CO₂ under green and sustainable conditions.

光催化二氧化碳还原代表了太阳能到化学能转换的一条有前途的途径，使碳中性燃料的可持续生产成为可能。由于复杂的多电子转移途径和相互竞争的反应中间体，实现对特定产物的高选择性仍然是一个主要挑战。本文以原位合成的mn掺杂ZIF-67为前驱体，基于“浸渍-热解”策略合成了mn掺杂Co3O4 （MMC）光催化剂。mof模板化方法可以使Mn均匀地结合到Co3O4晶格中，同时保持分层多孔结构，从而提高活性位点的可及性并调节催化剂的电子环境。客体锰的引入有效抑制了竞争性析氢反应。结果表明，优化后的2MMC催化剂的CO产量比未掺杂的Co3O4提高了12.8倍，并且可以在稀释的CO2中选择性地将CO2转化为纯水。光电化学表征表明客体锰掺杂加速了电荷分离动力学。原位辐照x射线光电子能谱、原位傅立叶变换红外光谱和理论计算揭示了锰介导的选择性促进*CO2和*CO中间体形成的途径。这项工作为绿色和可持续条件下CO2的选择性光催化转化提供了新的原子水平的见解。

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引用次数: 0

Mechanism of confinement enhancing enzyme intrinsic activity 禁闭增强酶内在活性的机制

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64827-3

Yufei Cao , Shuang Chen , Hui Liang , Junrong Yang , Wenyong Lou , Jun Ge

Enzymatic catalysis within surface- and volume-confined environments is common in biological cells or industrial applications. Despite their prevalence both in vivo and in vitro, a comprehensive mechanistic understanding of how these confinements tune the intrinsic activity of enzymes has remained elusive. Herein, we explore the role of confinement in shaping the activity of enzymes. Experiments show that the confinements induced by macromolecular crowding enhance lipase activity. To uncover the origin of the activity enhancement, thermodynamic activation parameters of lipase catalysis were calculated through extensive molecular dynamics (MD) and empirical valence bond (EVB) simulations. The EVB approach has proven to be an efficient method, enabling extensive sampling via MD and the evaluation of thermodynamic activation parameters for enzyme catalysis. Our findings reveal that confinement applied at the loop regions of lipase leads to higher intrinsic activities, and this effect depends on the degree of confinement. The lower free energy of activation originates from the gain of both enthalpy and entropy. Better preorganization of the active site and greater conformational space overlap between initial and transition states enhance lipase catalysis. We observe that the catalytic enhancement due to surface confinement is not exclusive to lipase but extends to PETase, highlighting its potential universality as a principle for enzyme design and engineering.

在生物细胞或工业应用中，表面和体积受限环境中的酶催化是常见的。尽管它们在体内和体外都很普遍，但对这些限制如何调节酶的内在活性的全面机制理解仍然难以捉摸。在这里，我们探索禁闭在塑造酶的活性中的作用。实验表明，由大分子拥挤引起的封闭使脂肪酶活性增强。为了揭示脂肪酶活性增强的原因，通过广泛的分子动力学（MD）和经验价键（EVB）模拟计算了脂肪酶催化的热力学激活参数。EVB方法已被证明是一种有效的方法，可以通过MD进行广泛的采样，并评估酶催化的热力学激活参数。我们的研究结果表明，在脂肪酶环区施加限制导致更高的内在活性，这种影响取决于限制的程度。激活自由能的降低源于焓和熵的增加。较好的活性位点预组织和初始态和过渡态之间较大的构象空间重叠增强了脂肪酶的催化作用。我们观察到，由于表面约束的催化增强不仅限于脂肪酶，而且延伸到PETase，突出了其作为酶设计和工程原理的潜在普遍性。

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引用次数: 0

Mn-doping induced phase segregation of air electrodes enables high-performance and durable reversible protonic ceramic cells 锰掺杂诱导的空气电极相偏析可以实现高性能和耐用的可逆质子陶瓷电池

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64907-2

Xiaofeng Chen, Yixuan Huang, Wanbin Lin, Jiaojiao Xia, Xirui Zhang, Wenjie Gong, Chuqian Jian, Hao Liu, Jiacheng Zeng, Jiang Liu, Yu Chen

Reversible protonic ceramic cells (R-PCCs) represent a highly promising energy conversion and storage technology, offering high efficiency at intermediate temperatures (400–700 °C). However, their commercialization is significantly impeded by the sluggish oxygen reaction kinetics on air electrodes. This work reports a Mn-doped PrBa_0.8Ca_0.2Co₂O_5+δ air electrode with a nominal composition of PrBa_0.8Ca_0.2Co_1.5Mn_0.5O_5+δ, which primarily segregates into a deficient double perovskite Pr_1.25Ba_0.5Ca_0.25Co_1.58Mn_0.42O_5+δ phase and a minor BaCo_0.6Mn_0.4O_3–δ hexagonal perovskite phase, as suggested by the X-ray diffraction refinement. The formation of Mn-doped nanocomposites substantially enhances the activities of oxygen reduction/evolution reactions, attributed to elevated oxygen vacancy concentrations and improved oxygen surface exchange and bulk diffusion capabilities, relative to the undoped PrBa_0.8Ca_0.2Co₂O_5+δ. The synergistic effect between the two phases may enhance electrochemical performance. Single cells incorporating these nanocomposite air electrodes achieve exceptional electrochemical performance at 700 °C: peak power density of 2.05 W cm^–2 in fuel cell (FC) mode and current density of –3.78 A cm^–2 at 1.3 V in electrolysis (EL) mode. Furthermore, promising durability is demonstrated during a FC test (100 h), an EL test (100 h), and a FC-EL cycling test (120 h) at 600 °C. This Mn-doping approach establishes an effective strategy for developing advanced air electrode materials.

可逆质子陶瓷电池（R-PCCs）是一种非常有前途的能量转换和存储技术，在中等温度（400-700°C）下具有很高的效率。然而，空气电极上缓慢的氧反应动力学严重阻碍了它们的商业化。本文报道了一种mn掺杂的PrBa0.8Ca0.2Co2O5+δ空气电极，其标称成分为PrBa0.8Ca0.2Co1.5Mn0.5O5+δ， x射线衍射细化表明，该电极主要偏析为缺乏的双钙钛矿pr1.25 ba0.5 ca0.25 co1.58 mn0.2o5 +δ相和少量的BaCo0.6Mn0.4O3 -δ六方钙钛矿相。相对于未掺杂的PrBa0.8Ca0.2Co2O5+δ， mn掺杂纳米复合材料的形成大大增强了氧还原/析出反应的活性，这是由于氧空位浓度升高，氧表面交换和体扩散能力增强。两相之间的协同作用可以提高电化学性能。采用这些纳米复合空气电极的单个电池在700°C下具有优异的电化学性能：燃料电池（FC）模式下的峰值功率密度为2.05 W cm-2，电解（EL）模式下的电流密度为-3.78 A cm-2，电压为1.3 V。此外，在600°C的FC测试（100小时）、EL测试（100小时）和FC-EL循环测试（120小时）中，耐久性也得到了证明。这种掺杂锰的方法为开发先进的空气电极材料建立了有效的策略。

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引用次数: 0

Composition regulation of iron-group transition metal chalcogenides for the oxygen electrocatalysis: Electronic structure and surface reconstruction 氧电催化用铁基过渡金属硫族化合物的组成调控：电子结构和表面重构

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64880-7

Haihong Zhong , Qianqian Xu , Weiting Yang , Nicolas Alonso-Vante , Yongjun Feng

Iron-group transition metal chalcogenides (IGTMCs) have emerged as promising electrocatalysts due to their tailorable electronic structures through composition engineering. This review summarizes the recent advancements in multi-component regulatory strategies employed in advanced IGTMC electrocatalysts, including anion substitution, cation doping, and the incorporation of zero-valent elements. Particular emphasis is placed on the roles of secondary and tertiary doping configurations, and chalcogen modulation in enhancing the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) of IGTMC electrocatalysts. Thus, regulating the electronic structure and optimizing the adsorption strengths on this family of materials are strategies to boost catalytic kinetics. Notably, dynamic surface reconstruction (e.g., oxidation) of IGTMC electrocatalysts during the OER has recently attracted significant attention. Advanced in-situ/operando characterization insights into reconstruction phenomenon of IGTMC electrocatalysts for OER process are critically analyzed. Finally, the challenges and prospects of IGTMC electrocatalysts for ORR/OER electrocatalysis are outlined.

铁基过渡金属硫族化合物（IGTMCs）由于其可定制的电子结构而成为一种很有前途的电催化剂。本文综述了近年来先进IGTMC电催化剂中多组分调控策略的研究进展，包括阴离子取代、阳离子掺杂和零价元素的掺入。特别强调了二级和三级掺杂构型的作用，以及硫调制在提高IGTMC电催化剂的氧还原反应（ORR）和析氧反应（OER）中的作用。因此，调节电子结构和优化在这类材料上的吸附强度是提高催化动力学的策略。值得注意的是，在OER过程中，IGTMC电催化剂的动态表面重建（例如氧化）最近引起了人们的极大关注。对OER过程中IGTMC电催化剂重构现象的原位/operando表征进行了批判性分析。最后，概述了IGTMC电催化剂在ORR/OER电催化方面面临的挑战和前景。

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引用次数: 0

Precise regulation of acid centers in different cavities of FER-zeolite via selective passivation to identify pentene monomolecular cracking reaction position 通过选择性钝化精确调控fe -沸石不同腔内酸中心，确定戊烯单分子裂解反应位置

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64887-X

Fang Li , Penghe Zhang , Yiran Wang , Yueming Liu , Mingyuan He

Precisely controlling acid center position in zeolites is still challenging. Pentene monomolecular cracking offers an ideal route to maximize ethylene and propylene yields simultaneously. To reveal the relationship between acid site distribution in FER-zeolite and pentene monomolecular cracking activity, this study proposes a novel strategy integrating pyridine pre-adsorption with K⁺ exchange modification to selectively shield acid sites within FER cages, while phosphorus modification is employed to selectively passivate acid sites in 10-MR channels and on the external surface. Adsorption infrared (IR) spectroscopy (CD₃CN-IR, Py-IR, and 2,6-DMPy-IR), and OH-IR characterization verified the selectivity and efficiency of these modification process. FER zeolites with distinct acid site distributions exhibit typical monomolecular cracking characteristics in pentene cracking, where the pentene cracking activity is linearly related to the acid density in the 10-MR channel and independent of the FER cage acidity. This result identifies 10-MR channel as primary pentene monomolecular cracking reaction position for the first time, providing a theoretical basis for designing zeolite catalysts that maximize ethylene and propylene production. The synergistic application of the pre-adsorption-K⁺ exchange modification strategy using different size basic molecules and phosphorus modification will provide an effective approach for precise control of acid site locations in zeolites with diverse pore/cavities architectures.

精确控制沸石中酸中心位置仍然具有挑战性。戊烯单分子裂解提供了一个理想的途径，以最大限度地提高乙烯和丙烯的产量同时。为了揭示fe -沸石中酸位点分布与戊烯单分子裂解活性之间的关系，本研究提出了一种新的策略，将吡啶预吸附与K +交换修饰结合起来，选择性地屏蔽FER笼内的酸位点，同时采用磷修饰选择性地钝化10-MR通道和外表面的酸位点。吸附红外光谱（CD3CN-IR， Py-IR和2,6- dmpy -IR）和OH-IR表征验证了这些修饰过程的选择性和效率。具有不同酸位分布的铁分子筛在戊烯裂解中表现出典型的单分子裂解特征，其中戊烯裂解活性与10-MR通道中的酸密度线性相关，与铁分子筛笼酸度无关。该结果首次确定了10-MR通道为伯戊烯单分子裂化反应位置，为设计最大化乙烯和丙烯产量的沸石催化剂提供了理论依据。不同大小碱性分子的预吸附- k +交换修饰策略和磷修饰的协同应用，将为精确控制不同孔/腔结构沸石中酸位点的位置提供有效的方法。

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引用次数: 0

From fundamental flaw to manageable parameter: Engineering salt precipitation out of acidic CO2RR for industrial viability 从根本缺陷到可管理的参数：工程盐沉淀从酸性CO2RR工业可行性

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64874-1

Genxiang Wang , Zhiwen Lu , Zhenhai Wen

Salt precipitation remains a persistent barrier to industrial CO₂ electrolysis. This Perspective analyzes transformative breakthroughs in acidic systems, elegantly connecting Sargent’s cation-focused interface engineering, Xia’s robust catalyst/reactor design, and Wang’s revolutionary acid humidification strategy into a cohesive industrial pathway. Based on this, we propose that integrating these approaches, combining acid-humidified feeds with durable catalysts and reactor designs, could establish a scalable route to industrial CO₂ electrolysis deployment powered by renewable electricity.

盐沉淀仍然是工业二氧化碳电解的持久障碍。本文分析了酸性系统的革命性突破，将Sargent以阳离子为中心的界面工程、Xia稳健的催化剂/反应器设计和Wang革命性的酸加湿策略巧妙地连接在一起，形成一条连贯的工业路径。基于此，我们建议整合这些方法，将酸加湿进料与耐用的催化剂和反应器设计相结合，可以建立一条可扩展的途径，以可再生电力为动力进行工业二氧化碳电解。

引用次数: 0

Innovative strategies and perspectives for enhancing photoelectrochemical water splitting: Physical field engineering 加强光电化学水分解的创新策略与展望：物理场工程

IF 17.7 1区化学 Q1 CHEMISTRY, APPLIED

Chinese Journal of Catalysis

Pub Date : 2026-02-01 Epub Date: 2026-02-03 DOI: 10.1016/S1872-2067(25)64894-7

Wenfeng Li, Guocheng Lv, Meng Liu, Fanyue Zhao, Zetian He, Guihong Li, Wenping Wang, Libing Liao, Daimei Chen

Photoelectrochemical (PEC) water splitting efficiently produces chemical fuels, yet persistent efficiency bottlenecks impede widespread deployment despite documented advances. In recent years, the introduction of external physical fields has emerged as a promising technique to remarkably improve the PEC performances of semiconductors both internally and externally. This review presents an in-depth exploration of the mechanisms underlying the utilization of thermal field (photothermal, pyroelectric effect), piezoelectric field (strain piezoelectricity, ferroelectric polarization), magnetic field (negative magnetoresistive effect, lorentz forces, spin polarization), and coupled fields in enhancing the synergistic effects of PEC water splitting, and subsequently analyzes their influence on the performance of PEC systems. It particularly emphasizes the underlying mechanisms that facilitate the strengthening of external fields on the excitation, transfer, and separation of carriers, as well as the enhancement of surface reactions. Additionally, we delve into the expansive prospects of externally assisted PEC water splitting, examining both its fundamental research implications and practical applications. Finally, we discuss the challenges encountered in its development and offer insights into potential future directions.

光电化学（PEC）水分解技术可以高效地生产化学燃料，尽管已有文献记载，但持续存在的效率瓶颈阻碍了该技术的广泛应用。近年来，引入外部物理场已成为一种有前途的技术，可以显着提高半导体内部和外部的PEC性能。本文深入探讨了利用热场（光热、热释电效应）、压电场（应变压电、铁电极化）、磁场（负磁阻效应、洛伦兹力、自旋极化）和耦合场增强PEC水裂解协同效应的机理，并分析了它们对PEC系统性能的影响。它特别强调了促进外场对载流子的激发、转移和分离以及表面反应增强的潜在机制。此外，我们深入研究了外部辅助PEC水裂解的广阔前景，研究了其基础研究意义和实际应用。最后，我们讨论了其发展中遇到的挑战，并提供了对潜在未来方向的见解。

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引用次数: 0