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学者姓名：张子重
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Abstract ：
Localized surface plasmon resonance (LSPR) on base-metal nanoparticles holds significant potential for applications in diverse fields owing to its capability for electric field enhancement. Nevertheless, the efficiency of single-energy conversion remains a limiting factor for LSPR applications. This study investigated the utilization of hot carriers, generated through the LSPR effect in copper nanoparticles (Cu NPs) supported on ZrO2, to enhance the performance of the thermal catalytic reverse water-gas shift (RWGS) reaction. Finite difference time domain simulations and Kelvin probe force microscopy (KPFM) tests demonstrated that LSPR induces a strong electric field, facilitating the excitation of hot carriers in Cu NPs. In-situ DRIFTS analysis revealed that hot electrons promote the formation of formate species (HCOO*) and their subsequent transformation into CO, identified as the rate-determining step. Furthermore, in-situ H2 pulse and quasi-in situ EPR analyses indicated that photo-assisted thermal conditions enhance the conversion of H2 into active hydrogen species (H* or H + ) on Cu NPs, promoting the generation of oxygen vacancies and the transformation of intermediates. Constrained density functional theory calculations further demonstrated that visible light irradiation reduces energy barriers, thereby increasing reaction efficiency. The findings provide valuable insights into the contribution of LSPR-induced hot electrons in advancing the RWGS reaction.
Keyword ：
Cu/ZrO 2 Cu/ZrO 2 Hot carriers Hot carriers Localized surface plasmon resonance Localized surface plasmon resonance Oxygen vacancies Oxygen vacancies Reverse water gas shift reaction Reverse water gas shift reaction
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| GB/T 7714 | Ni, Wenkang , Zhang, Xiaoyan , Yue, Xuanyu et al. Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 . |
| MLA | Ni, Wenkang et al. "Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles" . | SEPARATION AND PURIFICATION TECHNOLOGY 361 (2025) . |
| APA | Ni, Wenkang , Zhang, Xiaoyan , Yue, Xuanyu , Zhang, Zizhong , Zhang, Yongfan , Wang, Ke et al. Visible light enhanced thermocatalytic reverse water gas shift reaction via localized surface plasmon resonance of copper nanoparticles . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 . |
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Mimicking photosynthesis to convert CO2 and H2O into value-added chemicals represents an optimal approach to mitigate energy shortages and environmental pollution, and the development of highly efficient and selective photocatalysts for CO2 to CO conversion is essential for the effective utilization of CO2 resources. Herein, a novel 2D@0D InVO4@MnWO4 S-scheme heterojunction composite is successfully developed via an in situ hydrothermal method, achieving the conversion of CO2 into CO under visible light irradiation using H2O as a reducing agent, without any noble metal cocatalysts or sacrificial reagents. The CO generation rate over the optimal InVO4@MnWO4 composite reaches 6.20 mu mol g-1 h-1, which is approximately 4.50 times than that of InVO4. The enhanced photocatalytic performance is ascribed to the charge separation facilitated by the formation of an S-scheme heterojunction between InVO4 and MnWO4. This work is expected to provide a new insight for the design of highly selective photocatalysts for the conversion of CO2 to CO.
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| GB/T 7714 | Xiang, Wenzhuo , Xu, Guoyu , Xiao, Lujiang et al. Construction of a 2D@0D InVO4@MnWO4 S-scheme for efficient photocatalytic reduction of CO2 to CO [J]. | NEW JOURNAL OF CHEMISTRY , 2025 , 49 (9) : 3751-3758 . |
| MLA | Xiang, Wenzhuo et al. "Construction of a 2D@0D InVO4@MnWO4 S-scheme for efficient photocatalytic reduction of CO2 to CO" . | NEW JOURNAL OF CHEMISTRY 49 . 9 (2025) : 3751-3758 . |
| APA | Xiang, Wenzhuo , Xu, Guoyu , Xiao, Lujiang , Zhang, Zizhong , Ji, Tao , Su, Wenyue . Construction of a 2D@0D InVO4@MnWO4 S-scheme for efficient photocatalytic reduction of CO2 to CO . | NEW JOURNAL OF CHEMISTRY , 2025 , 49 (9) , 3751-3758 . |
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Photocatalytic water splitting on metal oxides often faces oxygen evolution inefficiency, reflecting the complex interplay of its two half-reactions. Strategies like heterojunctions, cocatalyst loading, or noble metal nano- particles addition have been explored to address this. Using gamma- Ga 2 O 3 nanosheets as a model, we uncovered the formation of-O-O- species as the key barrier to stoichiometric splitting. To tackle this, a strategy was devised, Sr-doping to inhibit surface peroxidation. The resultant Sr-doped gamma- Ga 2 O 3 (Sr-Ga2O3) significantly improved activity and stability, achieving balanced H2 and O2 production under 125 W mercury lamp light. Upon further enhancement with Rh/Cr2O3 cocatalyst via photoreduction, the Sr-Ga2O3/(Rh/Cr2O3) composite demonstrated a remarkable 173.3 mu mol & sdot;h-1 H2 and 86.7 mu mol & sdot;h-1 O2 evolution rate, 8.0 times higher than gamma- Ga 2 O 3 alone, with a 34.1 % quantum efficiency under 260 nm light. This represents a record performance for Ga2O3-based photo- catalytic water splitting. Mechanistically, Sr doping alters surface chemistry to favor direct oxygen release. Our study elucidates molecular-level insights into non-stoichiometric splitting mechanisms and offers a potent strategy to boost metal oxide photocatalysts' water-splitting efficiency.
Keyword ：
Photocatalytic stoichiometric water splitting Photocatalytic stoichiometric water splitting Sr-doped Sr-doped
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| GB/T 7714 | Shen, Jinni , Zhong, Yuhua , Lin, Jianhan et al. Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution [J]. | JOURNAL OF CATALYSIS , 2025 , 443 . |
| MLA | Shen, Jinni et al. "Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution" . | JOURNAL OF CATALYSIS 443 (2025) . |
| APA | Shen, Jinni , Zhong, Yuhua , Lin, Jianhan , Li, Haifeng , Qiu, Chengwei , Liu, Xu et al. Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution . | JOURNAL OF CATALYSIS , 2025 , 443 . |
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In heterogeneous photocatalysis, the dynamics of charge carriers holds particular significance for comprehending the underlying catalytic mechanism and designing highly efficient photocatalysts. The current technological challenge lies in how to maximize the behavior of carriers and enable them to unleash their potential in photocatalytic reactions. Herein, we present a novel Prussian blue analogue (PBA)-derived InFe-based oxide (denoted as InFe-x), which features internal Fe doping and an external crystalline/amorphous heterojunction, serving as an effective photocatalyst for photocatalytic reverse water gas shift (RWGS) reactions. Experiments and theoretical simulations have confirmed that doping Fe into In2O3 can alter the electronic and energy structure and achieve the spin polarization effect, thereby enhancing the intrinsic carrier generation and separation behavior; meanwhile, the formed Fe-In2O3/Fe2O3 S-scheme heterojunction establishes an internal built-in electric field and creates a new transport pathway for photogenerated carriers, which significantly inhibit the inherent photogenerated electron-hole recombination. Therefore, this "internal and external cultivation" strategy can fundamentally optimize and maximize the behavior of charge carriers, thereby significantly enhancing the photocatalytic CO2 hydrogenation performance.
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| GB/T 7714 | Guo, Yuhao , Guan, Qinhui , Li, Xingjuan et al. Internal and external cultivation: unleashing the potential of photogenerated carrier dynamics behaviors to boost photocatalytic CO2 hydrogenation [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (11) : 5539-5551 . |
| MLA | Guo, Yuhao et al. "Internal and external cultivation: unleashing the potential of photogenerated carrier dynamics behaviors to boost photocatalytic CO2 hydrogenation" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 11 (2025) : 5539-5551 . |
| APA | Guo, Yuhao , Guan, Qinhui , Li, Xingjuan , Zhao, Mengjun , Li, Na , Zhang, Zizhong et al. Internal and external cultivation: unleashing the potential of photogenerated carrier dynamics behaviors to boost photocatalytic CO2 hydrogenation . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (11) , 5539-5551 . |
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Controlling the crystallinity and microstructure of a semiconductor photocatalyst serves as an effective means to boost its photocatalytic performance through improving the charge transfer and separation, enhancing the light absorption, or maneuvering the surface reactions. Nevertheless, the internal pores in aerogel materials inevitably collapse during the traditional high temperature crystallization process, significantly reducing the porous structure and specific surface area (SSA). Herein, microsphere ZnO aerogels have been successfully fabricated for photoreduction of CO2 using a cooperative strategy of sol-gel method, solvothermal crystallization and cryodesiccation. The obtained aerogel has a large SSA and high crystallinity. Compared with the commercial ZnO powder, the ZnO aerogel microsphere exhibits about 4-fold increase in specific surface area, leading to an increased contact surface between the photocatalyst and the reactant. At the same time, ZnO aerogel with microsphere morphology possesses high light-harvesting and intrapore light reflecting capabilities, demonstrating enhanced optical utilization. Modulation of the crystallinity of ZnO aerogel facilitated the incorporation of defect engineering (zinc defects (Zni) and oxygen vacancies (Vo)). As a result, ZnO aerogel microsphere exhibits a 5-fold higher products production rate than ZnO powder for photocatalytic CO2 reactions due to the synergistic effect of appropriate crystallinity and microsphere appearance. It is hoped that this work may provide some insights to tune the catalyst performance through crystallinity and morphology.
Keyword ：
CO2 reduction reaction CO2 reduction reaction Crystallization Crystallization Photocatalysis Photocatalysis Solvothermal Solvothermal ZnO aerogel microspheres ZnO aerogel microspheres
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| GB/T 7714 | Xu, Xiaochao , Zou, Jiaxin , Xiao, Zhen et al. Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction [J]. | FUEL , 2025 , 398 . |
| MLA | Xu, Xiaochao et al. "Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction" . | FUEL 398 (2025) . |
| APA | Xu, Xiaochao , Zou, Jiaxin , Xiao, Zhen , Zhang, Jiangjie , Wang, Bing , Jiang, Jianing et al. Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction . | FUEL , 2025 , 398 . |
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Employing photocatalytic technology to transform CO2 into valuable fuels is considered a promising solution for addressing the exacerbated greenhouse effect and energy crisis. The development of photocatalysts featuring superior charge separation efficiency is pivotal for the widespread implementation of photocatalytic CO2 reduction technologies. Herein, zero-dimensional (0D) NixP nanoparticles are anchored onto two-dimensional (2D) LaTiO2N nanosheets by a photo-deposition method, and a NixP/LaTiO2N Schottky junction composite with excellent photocatalytic CO2 reduction performance is constructed. The optimal NixP/LaTiO2N composite achieves CO and CH4 yields of 9.39 and 4.15 mu mol g-1 h-1, respectively, with the utilized photoelectron number (UPN) reaching 51.98 mu mol g-1, which is approximately 9.7 times higher than that of LaTiO2N alone. The improved photocatalytic performance of the composites can be attributed to the formation of Schottky junctions, which effectively suppress the recombination of photogenerated carriers. This study provides a new idea for the development of 0D/2D Schottky junction photocatalysts.
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| GB/T 7714 | Xu, Guoyu , Chen, Yanan , Lin, Peiling et al. Construction of a 0D/2D NixP/LaTiO2N Schottky junction photocatalyst for efficient visible-light-driven photocatalytic CO2 reduction [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2025 , 15 (6) : 2027-2033 . |
| MLA | Xu, Guoyu et al. "Construction of a 0D/2D NixP/LaTiO2N Schottky junction photocatalyst for efficient visible-light-driven photocatalytic CO2 reduction" . | CATALYSIS SCIENCE & TECHNOLOGY 15 . 6 (2025) : 2027-2033 . |
| APA | Xu, Guoyu , Chen, Yanan , Lin, Peiling , Zhang, Zizhong , Ji, Tao , Su, Wenyue . Construction of a 0D/2D NixP/LaTiO2N Schottky junction photocatalyst for efficient visible-light-driven photocatalytic CO2 reduction . | CATALYSIS SCIENCE & TECHNOLOGY , 2025 , 15 (6) , 2027-2033 . |
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The photocatalytic nonoxidative coupling of methane (CH4) is crucial for sustainable energy production and chemical synthesis, however, a key challenge in advancing this process lies in the development of efficient and highly selective catalytic systems. In this study, we employ an in situ thermally induced strategy to promote the in-situ growth of oxygen vacancies (VO) for constructing a high-density In-VO-In-OH frustrated Lewis pairs (FLP) on Ag/In(OH)3-InOOH (Ag/InOxHy). Our results demonstrate that FLP can effectively polarize C-H bonds, while Ag nanoparticles serve as electron acceptors, significantly reducing the recombination of photogenerated carriers and enhancing the catalytic performance of methane coupling. Benefiting from the high density of FLP and photothermal synergistic effect, we achieve a remarkable C2H6 yield of 339.2 mu mol gcat flow methane atmosphere. Notably, in-situ electron paramagnetic resonance analysis not only validates this innovative strategy but also reveals a new mechanism of oxygen vacancy recycling which showcases its great potential to advance other photocatalytic processes.
Keyword ：
High-density frustrated Lewis pairs High-density frustrated Lewis pairs In(OH)3 /InOOH In(OH)3 /InOOH In-situ growth of oxygen vacancies In-situ growth of oxygen vacancies Non-oxidative coupling of methane Non-oxidative coupling of methane Photothermal effect Photothermal effect
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| GB/T 7714 | Yan, Ziyuan , Li, Xiaoning , Guan, Xinwei et al. Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy [J]. | JOURNAL OF CATALYSIS , 2025 , 447 . |
| MLA | Yan, Ziyuan et al. "Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy" . | JOURNAL OF CATALYSIS 447 (2025) . |
| APA | Yan, Ziyuan , Li, Xiaoning , Guan, Xinwei , Wang, Zhaoliang , Shen, Jinni , Yan, Tingjiang et al. Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy . | JOURNAL OF CATALYSIS , 2025 , 447 . |
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Photocatalytic CO2 reduction comprises two coupled half-reactions: CO2 reduction and H2O oxidation. Efficient coupling of these reactions maximizes the utilization of photogenerated electrons and holes, enhancing CO2 conversion and product selectivity. In this study, sulfur-deficient VS-Zn3In2S6 (VS-ZIS) catalysts were synthesized via an ethylene glycol solvothermal method, followed by anchoring Fe single-atom sites (Fe/VS-ZIS) to facilitate CO2 photoreduction using H2O as proton source. The 1 %Fe/VS-ZIS exhibited exceptional performance, with a CO production rate of 88.6 μmol·g−1·h−1 and 97 % selectivity. Experimental and DFT results revealed that VS functioned as reductive sites to strengthen CO2 adsorption and activation, while Fe single atoms (SAs) served as oxidative sites to facilitate H2O dissociation for proton supply. Fe SAs also induced spin polarization to enhance IEF, thereby suppressing photogenerated charges recombination at redox sites. Meanwhile, Fe SAs reduced COOH* formation energy barrier and lowered CO desorption temperature, improving CO selectivity. The constructed dual active sites synergistically enhanced the overall photocatalytic CO2 reduction performance. This work offers new technical pathways for designing redox dual-active sites to boost the overall photocatalytic CO2 reduction efficiency. © 2025 Elsevier B.V.
Keyword ：
Photocatalytic activity Photocatalytic activity Photodissociation Photodissociation Redox reactions Redox reactions
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| GB/T 7714 | Zhang, Xiaoyan , Ni, Wenkang , He, Peihang et al. Dual redox-active sites with synergistic spin polarization effect to facilitate overall CO2 photoreduction with H2O [J]. | Chemical Engineering Journal , 2025 , 514 . |
| MLA | Zhang, Xiaoyan et al. "Dual redox-active sites with synergistic spin polarization effect to facilitate overall CO2 photoreduction with H2O" . | Chemical Engineering Journal 514 (2025) . |
| APA | Zhang, Xiaoyan , Ni, Wenkang , He, Peihang , Wang, Zhijie , Wang, Ke , Zhang, Zizhong et al. Dual redox-active sites with synergistic spin polarization effect to facilitate overall CO2 photoreduction with H2O . | Chemical Engineering Journal , 2025 , 514 . |
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H2 and O2 evolutions occur simultaneously for conventional particulate photocatalytic overall water splitting (PPOWS), leading to a significant backward reaction and the formation of an explosive H2/O2 gas mixture. This is an issue that must be addressed prior to industrialization of PPOWS. Here, a convenient, cost-effective, and scalable concept is introduced to uncouple hydrogen and oxygen production for PPOWS. Based on this idea, a three-component photocatalyst, Co(5 %)-HPCN/(rGO/Pt), is constructed, consisting of a photoresponsive chip (HPCN), a H2 evolution cocatalyst (rGO/Pt), and a cobalt complex capable of reversibly binding O2 (Co), to achieve the decoupling of PPOWS under alternating UV and visible light irradiations. The asynchronous O2 and H2 evolution strategy have considerable flexibility regarding the photocatalyst structure and light sources suitable for PPOWS.
Keyword ：
carbon nitride chips carbon nitride chips overall water splitting overall water splitting photocatalytic photocatalytic PPOWS decoupling PPOWS decoupling reaction mechanism reaction mechanism
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| GB/T 7714 | Liu, Dan , Xu, Huihui , Shen, Jinni et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
| MLA | Liu, Dan et al. "Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 9 (2025) . |
| APA | Liu, Dan , Xu, Huihui , Shen, Jinni , Wang, Xun , Qiu, Chengwei , Lin, Huaxiang et al. Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (9) . |
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CH3OH is the most desired product of photocatalytic CH4 conversion. The prominent metal-decorated photocatalyst is challenging in both high yield and selectivity for CH3OH products due to over-oxidation by center dot OH mechanism. Here, interstitial Zn is fabricated into ZniO to induce the formation of Zn atom island for rapid single electron reduction of O2 into center dot OOH instead of center dot OH for the selective combination with methyl into CH3OOH. AuPd alloy is simultaneously decorated on ZniO surface for tuning CH3OOH adsorption and reduction into CH3OH. The synergy of Zn atom island and AuPd alloy achieve a tandem reaction pathway (CH4 -> CH3OOH -> CH3OH) for an unprecedented CH3OH yield of 2444 mmol gAuPd-1 h-1 (or 8800 mu mol gcat-1 h-1) with 98.3% selectivity, which bypasses the center dot OH mechanism for tuning the high selectivity of CH3OH. An apparent quantum efficiency of 18.53% at 370 nm for CH4 conversion are super to the reported photocatalytic systems. Thus, this work provides the new strategy of the synergetic atom island and metal alloy photocatalysts through a tandem reaction pathway to mediate the photocatalytic selective oxidation of CH4 into the desired CH3OH.
Keyword ：
atom island atom island AuPd alloy AuPd alloy methanol selectivity methanol selectivity photocatalysis photocatalysis tandem reaction tandem reaction
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| GB/T 7714 | Xiao, Zhen , Shen, Jinni , Jiang, Jianing et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Xiao, Zhen et al. "Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Xiao, Zhen , Shen, Jinni , Jiang, Jianing , Zhang, Jiangjie , Liang, Shuqi , Han, Shitong et al. Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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