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学者姓名：付贤智
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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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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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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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Persulfate-based advanced oxidation technology, due to its high efficiency, controllability, and safety, shows great potential for the deep removal of organic pollution, yet its mineralization efficiency is hindered by the lack of synergy between radical and nonradical pathways. Herein, we present defective carbon nitride (DCN) as a highly efficient peroxymonosulfate (PMS) activation catalyst that couples nonradical aggregation with radical mineralization. The tailored electronic structure of the DCN framework enhances visible-light absorption, photogenerated charge separation, and electron transfer ability due to a built-in electric field. DCN effectively interacts with PMS to rapidly accumulate pollutants from the bulk solution onto the catalyst surface via an electron-transfer pathway. Simultaneously, the accumulated pollutants undergo in-situ decomposition by center dot SO4- radicals formed on the catalyst surface under visible light irradiation, achieving a remarkable 98 % mineralization ratio. The mixed-pathway process demonstrates excellent cyclic stability and environmental robustness. This study introduces a novel strategy to enhance the catalytic oxidation performance of metal-free catalysts by controlling persulfate activation pathways for water decontamination.
Keyword ：
Carbon nitride Carbon nitride Peroxymonosulfate Peroxymonosulfate Photocatalysis Photocatalysis Pollutant mineralization Pollutant mineralization Synergistic Synergistic
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| GB/T 7714 | Ming, Hongbo , Ruan, Wenqi , Yuan, Xiaoying et al. Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 360 . |
| MLA | Ming, Hongbo et al. "Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization" . | SEPARATION AND PURIFICATION TECHNOLOGY 360 (2025) . |
| APA | Ming, Hongbo , Ruan, Wenqi , Yuan, Xiaoying , Cheng, Jiajia , Yang, Can , Hou, Yidong et al. Defective carbon nitride-Mediated peroxymonosulfate activation: Synergistic radical and nonradical pathways for enhanced pollutant mineralization . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 360 . |
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Photocatalytic ozonation holds promise for advanced water purification, yet its development has been hindered by a limited understanding of ozone activation mechanisms and its related photogenerated electron transfer dynamics. Herein, we employed in-situ DRIFTS and Raman spectroscopy to elucidate the distinct adsorption and activation behaviors of ozone (O3) on the {001} and {110} crystal facets of Bi2O2CO3 (BOC) nanosheets. BOC-{001} demonstrates superior photocatalytic ozonation performance, with 85% phenol mineralization and excellent durability, significantly outperforming the 53% mineralization rate of BOC-{110}. This enhanced activity is attributed to non-dissociative ozone adsorption and favorable adsorption energy over {001} facet, which facilitate the one-electron O3 reduction pathway. Furthermore, crystal facet engineering strengthens the built-in electric field, promoting exciton dissociation and the generation of localized charge carriers. The synergistic effects of optimized electron availability and ozone adsorption significantly boost the production of reactive oxygen species. These findings provide a deeper understanding of the critical roles of O3 adsorption and electron transfer in radical generation, which could provide some guidance for the strategic development of highly effective photocatalytic ozonation catalysts. © 2025 Dalian Institute of Chemical Physics, the Chinese Academy of Sciences
Keyword ：
Air cleaners Air cleaners Boron compounds Boron compounds Nanosheets Nanosheets Ozonization Ozonization Photocatalysis Photocatalysis Selenium compounds Selenium compounds
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| GB/T 7714 | Yang, Yang , Yang, Zhou , Lai, Zhiming et al. Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism [J]. | Chinese Journal of Catalysis , 2025 , 72 : 143-153 . |
| MLA | Yang, Yang et al. "Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism" . | Chinese Journal of Catalysis 72 (2025) : 143-153 . |
| APA | Yang, Yang , Yang, Zhou , Lai, Zhiming , Yang, Can , Hou, Yidong , Tao, Huilin et al. Crystal facet engineering of Bi2O2CO3 nanosheets to enhance photocatalytic ozonation: Unraveling ozone adsorption and electron transfer mechanism . | Chinese Journal of Catalysis , 2025 , 72 , 143-153 . |
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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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光催化臭氧化技术作为一种新兴的高级氧化工艺,相较于传统臭氧化技术,展现出显著提升的氧化效能与环境治理潜力.光催化臭氧化技术的创新之处在于将光催化与臭氧化进行耦合,通过光生载流子(e-与h+)驱动臭氧活化,生成羟基自由基(•OH)和超氧自由基(•O2-)等高活性氧物种,形成多路径氧化网络,实现污染物的快速降解与深度矿化.相关研究表明,该技术可显著降低臭氧投加量并有效控制残留臭氧浓度,兼具经济性与环境友好性.然而,光生电子参与的臭氧还原过程涉及吸附-解离-自由基级联反应等诸多复杂步骤,其在分子层面的作用机制仍有待进一步明确,这已然成为制约该技术优化的关键科学难题. 针对光催化臭氧化反应中臭氧活化机制的复杂性,本文采用晶面工程策略,深入探究并阐明了催化剂表面结构对臭氧吸附与活化行为所起到的决定性影响.以层状Bi2O2CO3(BOC)为模型催化剂,研究发现{110}晶面与{001}晶面凭借差异化的原子排布,能够调控臭氧吸附特性与反应路径.BOC-{110}吸附臭氧能力强,可直接解离O3为表面原子氧(*O)与氧气(O2),主导表面直接氧化路径;而BOC-{001}则具有适中的O3吸附能力,有利于光生电子向O3转移,形成•O3-中间体,经质子化作用进一步生成•OH与O2,主导自由基间接氧化路径.原位光谱表征证实了这种晶面依赖的臭氧活化差异:红外光谱监测到吸附在BOC-{001}表面上臭氧(*O3)在光照条件下被迅速消耗;拉曼光谱则观察到BOC-{110}表面上*O的累积.此外,晶面工程还能调控光催化剂的内建电场,暴露{001}晶面促进激子的解离以及载流子的分离,进一步加速了光生电子活化臭氧的动力学过程,产生更多羟基自由基.因此,BOC-{001}在光催化臭氧化过程中表现出优异的苯酚矿化率(85%),明显优于BOC-{110}(53%),并保持良好的循环稳定性. 综上,晶面工程在光催化臭氧化体系中的创新性应用,为高性能催化剂的构筑提供了全新的视角.通过精准调控催化剂的暴露晶面与表面活性位点,可实现臭氧吸附强度、光生载流子迁移路径及活性自由基定向生成动力学的多维度优化.电荷分离效率与臭氧活化效率的同步提升,成功突破了光催化体系中单电子活化臭氧动力学的速率限制,进而有望实现难降解有机污染物的深度矿化.
Keyword ：
Bi2O2CO3 Bi2O2CO3 光催化臭氧化 光催化臭氧化 吸附构型 吸附构型 晶面工程 晶面工程 臭氧活化 臭氧活化
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| GB/T 7714 | 杨洋 , 杨洲 , 赖志明 et al. Bi2O2CO3纳米片晶面工程增强光催化臭氧化:揭示臭氧吸附与电子转移机制 [J]. | 催化学报 , 2025 , 72 (5) : 143-153 . |
| MLA | 杨洋 et al. "Bi2O2CO3纳米片晶面工程增强光催化臭氧化:揭示臭氧吸附与电子转移机制" . | 催化学报 72 . 5 (2025) : 143-153 . |
| APA | 杨洋 , 杨洲 , 赖志明 , 阳灿 , 侯乙东 , 陶慧琳 et al. Bi2O2CO3纳米片晶面工程增强光催化臭氧化:揭示臭氧吸附与电子转移机制 . | 催化学报 , 2025 , 72 (5) , 143-153 . |
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A prepared p -type PdO/n-type TiO2 junction was prepared as the catalyst for photocatalytic hydrogen evolution from formic acid (FA). It was found that PdO/TiO2 exhibited 1298 -fold higher activity than TiO2 under ultraviolet and visible light irradiation at room temperature. Multiple characterization techniques were utilized to demonstrate that doping PdO into TiO2 can regulate the Fermi level of the sample and the adsorption behavior of FA, resulting in different electron transfer behavior between FA and PdO/TiO2 compared to that between FA and TiO2. Oxygen vacancies acted as electron donors to deliver photogenerated electrons from TiO2 to the adsorbed bidentate FA, which increased the electron density on the O atom of FA and led to the formation of activated monodentate FA. This activated FA was more easily oxidized by the holes in PdO generated by visible light, leading to the production of H2 and CO2. The mode of adsorption associated with the Pd2+ site is the key factor in driving this reaction and leading to the reversible electron transfer phenomenon. This study provides a new promising route for the design of photocatalysts for self -decomposition reactions.
Keyword ：
Adsorption behavior Adsorption behavior After photocatalysis After photocatalysis Electron transfer Electron transfer Hydrogen production Hydrogen production PdO/TiO2 PdO/TiO2 Photocatalysis formic acid Photocatalysis formic acid
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| GB/T 7714 | Wang, Hong , Wang, Zhongming , Zhang, Zizhong et al. Enhanced photocatalytic hydrogen production from formic acid with reversible electron transfers in PdO/TiO2 [J]. | FUEL , 2024 , 362 . |
| MLA | Wang, Hong et al. "Enhanced photocatalytic hydrogen production from formic acid with reversible electron transfers in PdO/TiO2" . | FUEL 362 (2024) . |
| APA | Wang, Hong , Wang, Zhongming , Zhang, Zizhong , Fan, Yaming , Fu, Xianzhi , Dai, Wenxin . Enhanced photocatalytic hydrogen production from formic acid with reversible electron transfers in PdO/TiO2 . | FUEL , 2024 , 362 . |
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The construction of photothermal catalysts to provide advanced oxidation ability and stability is a great challenge for eliminating volatile organic compounds (VOCs) during the photothermal catalytic process. Herein, a bimetallic modification method was proposed to synthesize Pd/Fe-TiO2. Under ultraviolet-visible (UV-Vis) light irradiation with the intensity of 610 mW/cm(2), the optimal 0.7 wt% Pd/0.4 wt% Fe-TiO2 catalyst of which surface was detected at the temperature of 165 C can achieve a toluene conversion of 94 % and a CO2 yield of 87 %, respectively. Based on the results of in-situ DRIFTS, quasi-situ EPR, XPS, and O-2-TPD tests, it was found that two distinct types of Pd and Fe active sites not only generated reactive oxygen species (ROS) but also adsorbed toluene and intermediate species, which promoted the degradation of toluene. It is proposed that there be an electron transfer behavior between Fe and Pd nanoparticles, resulting in a synergistic interaction of the two metals. This study shows that creating bimetallic modification catalysts is an efficient method for eliminating VOCs through photothermal catalysis.
Keyword ：
Bimetallic modification Bimetallic modification Oxidative degradation Oxidative degradation Photothermal catalysis Photothermal catalysis ROS ROS Toluene Toluene
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| GB/T 7714 | Fan, Shipeng , Luo, Songyu , Wang, Yun et al. TiO2-based Pd/Fe bimetallic modification for the efficient photothermal catalytic degradation of toluene: The synergistic effect of •O2- and •OH species [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 336 . |
| MLA | Fan, Shipeng et al. "TiO2-based Pd/Fe bimetallic modification for the efficient photothermal catalytic degradation of toluene: The synergistic effect of •O2- and •OH species" . | SEPARATION AND PURIFICATION TECHNOLOGY 336 (2024) . |
| APA | Fan, Shipeng , Luo, Songyu , Wang, Yun , Yue, Xuanyu , Zheng, Duojia , Zhang, Zizhong et al. TiO2-based Pd/Fe bimetallic modification for the efficient photothermal catalytic degradation of toluene: The synergistic effect of •O2- and •OH species . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 336 . |
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Halogenated methane serves as a universal platform molecule for building high-value chemicals. Utilizing sodium chloride solution for photocatalytic methane chlorination presents an environmentally friendly method for methane conversion. However, competing reactions in gas-solid-liquid systems leads to low efficiency and selectivity in photocatalytic methane chlorination. Here, an in situ method is employed to fabricate a hydrophobic layer of TaOx species on the surface of NaTaO3. Through in-situ XPS and XANES spectra analysis, it is determined that TaOx is a coordination unsaturated species. The TaOx species transforms the surface properties from the inherent hydrophilicity of NaTaO3 to the hydrophobicity of TaOx/NaTaO3, which enhances the accessibility of CH4 for adsorption and activation, and thus promotes the methane chlorination reaction within the gas-liquid-solid three-phase system. The optimized TaOx/NaTaO3 photocatalyst has a good durability for multiple cycles of methane chlorination reactions, yielding CH3Cl at a rate of 233 mu mol g(-1) h(-1) with a selectivity of 83%. In contrast, pure NaTaO3 exhibits almost no activity toward CH3Cl formation, instead catalyzing the over-oxidation of CH4 into CO2. Notably, the activity of the optimized TaOx/NaTaO3 photocatalyst surpasses that of reported noble metal photocatalysts. This research offers an effective strategy for enhancing the selectivity of photocatalytic methane chlorination using inorganic chlorine ions.
Keyword ：
hydrophobicity hydrophobicity methane chlorination methane chlorination photocatalysis photocatalysis TaOx TaOx ultrathin layer ultrathin layer
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| GB/T 7714 | Li, Dongmiao , Lin, Min , Zhang, Jiangjie et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine [J]. | SMALL , 2024 , 20 (38) . |
| MLA | Li, Dongmiao et al. "Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine" . | SMALL 20 . 38 (2024) . |
| APA | Li, Dongmiao , Lin, Min , Zhang, Jiangjie , Qiu, Chengwei , Chen, Hui , Xiao, Zhen et al. Hydrophobic TaOx Species Overlayer Tuning Light-Driven Methane Chlorination with Inorganic Chlorine . | SMALL , 2024 , 20 (38) . |
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