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学者姓名：戴文新
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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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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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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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CO2 conversion with pure H2O into CH3OH and O-2 driven by solar energy can supply fuels and life-essential substances for extraterrestrial exploration. However, the effective production of CH3OH is significantly challenging. Here we report an organozinc complex/MoS2 heterostructure linked by well-defined zinc-sulfur covalent bonds derived by the structural deformation and intensive coupling of dx 2 - y2(Zn)-p(S) orbitals at the interface, resulting in distinctive charge transfer behaviors and excellent redox capabilities as revealed by experimental characterizations and firstprinciple calculations. The synthesis strategy is further generalized to more organometallic compounds, achieving various heterostructures for CO2 photoreduction. The optimal catalyst delivers a promising CH3OH yield of 2.57 mmol gcat-1 h(-1) and selectivity of more than 99.5%. The reverse water gas shift mechanism is identified for methanol formation. Meanwhile, energy-unfavorable adsorption of methanol on MoS2, where the photogenerated holes accumulate, ensures the selective oxidation of water over methanol.
Keyword ：
CO2 photoreduction CO2 photoreduction extraterrestrial synthesis extraterrestrial synthesis methanol methanol strong metal-supportinteractions strong metal-supportinteractions two-dimensional heterostructures two-dimensional heterostructures
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| GB/T 7714 | Cheng, Ming , Cao, Ning , Wang, Zhi et al. Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O [J]. | ACS NANO , 2024 , 18 (15) : 10582-10595 . |
| MLA | Cheng, Ming et al. "Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O" . | ACS NANO 18 . 15 (2024) : 10582-10595 . |
| APA | Cheng, Ming , Cao, Ning , Wang, Zhi , Wang, Ke , Pu, Tiancheng , Li, Yukun et al. Strain-Induced Self-Assembly at Interface of Two-Dimensional Heterostructures Boosts CO2 Reduction to Methanol by H2O . | ACS NANO , 2024 , 18 (15) , 10582-10595 . |
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Photocatalytic oxidative coupling of methane (POCM) is a direct way for the methane transformation into >= C2 alkanes. However, the typical oxygen activation path often leads to the formation of strong oxidizing superoxide radical (O-2(-)) species, which makes the whole reaction face serious selectivity problems. Herein, we constructed N and oxygen vacancy dual active sites on TiO2{001} nanosheets (TiO2-NVo) to regulate the oxygen activation pathway and achieve a high activity and selectivity of photocatalytic OCM. Compared with ordinary Au/TiO2{001} nanosheets, the alkane yields of Au/TiO2-NVo are increased from 16 mu mol h(-1) to 32 mu mol h(-1), and the selectivity of alkanes increased from 61% to 93%. The performance is superior when compared with the reported till date in photocatalytic OCM in batch reactors. The superior performance originates from the unique N-V-o dual active sites for synergistically cleaving the detrimental O-2(-) into desirable mono-oxygen active species (O-) to suppress undesired overoxidation reaction. The formed O- species from O-2(-) dissociation, in turn, is active for the selective H abstraction of CH4 into center dot CH3 to improve the subsequent C-C coupling reaction on the Au nanocluster surface. This work provides a new approach of O-2 dissociation to address the overoxidation of methane in an aerobic environment for achieving highly selective CH4 conversion.
Keyword ：
dual sites dual sites high selectivity high selectivity O-2 dissociation O-2 dissociation oxidative coupling of methane oxidative coupling of methane photocatalysis photocatalysis
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| GB/T 7714 | Zhang, Jiangjie , Zhang, Junhui , Shen, Jinni et al. Regulation of Oxygen Activation Pathways to Optimize Photocatalytic Methane Oxidative Coupling Selectivity [J]. | ACS CATALYSIS , 2024 , 14 (6) : 3855-3866 . |
| MLA | Zhang, Jiangjie et al. "Regulation of Oxygen Activation Pathways to Optimize Photocatalytic Methane Oxidative Coupling Selectivity" . | ACS CATALYSIS 14 . 6 (2024) : 3855-3866 . |
| APA | Zhang, Jiangjie , Zhang, Junhui , Shen, Jinni , Li, Dongmiao , Long, Jinlin , Dai, Wenxin et al. Regulation of Oxygen Activation Pathways to Optimize Photocatalytic Methane Oxidative Coupling Selectivity . | ACS CATALYSIS , 2024 , 14 (6) , 3855-3866 . |
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Photocatalytic hydrogen production from formic acid (FA) is a daunting challenge, yet an essential task forthe development of hydrogen energy. In this study, a p-NiO/n-TiO2 heterojunction incorporating 7-nm metallic Ni was fabricated, which demonstrated a remarkable localized surface plasmon resonance (LSPR) effect. Notably, 5 wt% Ni/TiO2 exhibited 1271 -fold higher photocatalytic activity (2416 mu mol center dot g- 1 center dot h-1) than TiO2 alone under light radiation at room temperature. The experimental investigations revealed the excitation of distinct components via irradiation by different light sources. Visible light -driven hydrogen production was predominantly influenced by the LSPR-induced hot electrons and holes effects of Ni. Further, FA molecules simultaneously lost and accepted electrons at the Ni0-Ti3+ and Ni0-O2- sites, respectively, generating a bidirectional electron transfer behavior with "valley -shaped" gas -sensitive responses, which was crucial to boost the activity. Moreover, the photocatalytic activity was mainly attributed to the heterojunction and defects structure under UV light irradiation, and Ti3+, VOs, and O2- as adsorption sites for FA. Thus, the synergistic interplay among different light sources could effectively boost the photocatalytic hydrogen production performance. Significantly, this research reveals that the LSPR effect of metallic Ni can effectively regulate electron transfer behavior and enhance visible light -driven photocatalytic activity.
Keyword ：
Adsorption behavior Adsorption behavior Electron transfer Electron transfer formic acid formic acid Localized surface plasmon resonance (LSPR) Localized surface plasmon resonance (LSPR) Metallic Ni Metallic Ni Photocatalysis hydrogen production from Photocatalysis hydrogen production from
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| GB/T 7714 | Wang, Zhongming , Huang, Xiaoqian , Jia, Yong et al. Localized surface plasmon resonance-induced bidirectional electron transfer of formic acid adsorption for boosting photocatalytic hydrogen production on Ni/TiO2 [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
| MLA | Wang, Zhongming et al. "Localized surface plasmon resonance-induced bidirectional electron transfer of formic acid adsorption for boosting photocatalytic hydrogen production on Ni/TiO2" . | CHEMICAL ENGINEERING JOURNAL 482 (2024) . |
| APA | Wang, Zhongming , Huang, Xiaoqian , Jia, Yong , Guo, Lina , Wang, Hong , Dai, Wenxin . Localized surface plasmon resonance-induced bidirectional electron transfer of formic acid adsorption for boosting photocatalytic hydrogen production on Ni/TiO2 . | CHEMICAL ENGINEERING JOURNAL , 2024 , 482 . |
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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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