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学者姓名：戴文新
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Abstract ：
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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Upcycling of NO into NH3 provided a win-win strategy for NO purification and NH3 production. In this work, we reported an approach for NH3 production via photo-assisted thermalcatalytic NO and H2O reduction by CO at low temperature and atmospheric pressure. Herein, a Pd/TiO2 model catalyst with electron-enriched Pd and oxygen vacancies dual active sites was applied. The results showed that full NO conversion was realized only at 120 degrees C, and a beyond 55.0% NH3 selectivity could be obtained below 180 degrees C over Pd/TiO2. A series of collective spectroscopic and theoretical investigations revealed that CO adsorbed at Pd site and H2O dissociated at interfacial oxygen vacancies would first interact to in situ generate active *H species, and then NO also adsorbed at interfacial oxygen vacancies was gradually hydrogenated by *H to produce NH3. Light irradiation further reinforced this process by promoting oxygen vacancies formation and electron transfer for enhancing CO and NO activation and H2O dissociation. This work provides a valuable insight into NH3 production via photothermal catalytic NO and H2O reduction by CO.
Keyword ：
NH3 production NH3 production NO and H2O reduction NO and H2O reduction Oxygen vacancies Oxygen vacancies Pd/TiO2 Pd/TiO2 Photothermal catalysis Photothermal catalysis
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| GB/T 7714 | Cheng, Gang , Zou, Junhua , Song, Xinjie et al. NH3 synthesis via photo-assisted thermalcatalytic NO and H2O reduction by CO over Pd/TiO2: Synergistic effects of Pd and oxygen vacancies [J]. | MOLECULAR CATALYSIS , 2025 , 578 . |
| MLA | Cheng, Gang et al. "NH3 synthesis via photo-assisted thermalcatalytic NO and H2O reduction by CO over Pd/TiO2: Synergistic effects of Pd and oxygen vacancies" . | MOLECULAR CATALYSIS 578 (2025) . |
| APA | Cheng, Gang , Zou, Junhua , Song, Xinjie , Tang, Hongmei , Gong, Qing , Liu, Hongxian et al. NH3 synthesis via photo-assisted thermalcatalytic NO and H2O reduction by CO over Pd/TiO2: Synergistic effects of Pd and oxygen vacancies . | MOLECULAR CATALYSIS , 2025 , 578 . |
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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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NO-to-NH3 conversion using H2O enables eco-friendly ammonia synthesis that simultaneously reduces pollutants and recovers resources. However, existing catalytic systems still face key challenges such as high reaction temperatures, insufficient utilization of hydrogen species and low NH3 selectivity. In this work, Pd-Fe/CeO2 catalyst utilizes Pd to provide CO/NO adsorption sites, achieving 100 % NO conversion at 150 degrees C with significantly reduced reaction temperature. XPS confirmed that the constructed Pd-O-Fe interface increased the electron density on the Pd surface, and in-situ DRIFTS demonstrated that the migration of H* from the Pd to the Fe sites enhanced the utilization of hydrogen species. In addition, the lattice distortion due to the introduction of Fe sites generates more oxygen vacancies (OVs), which promoted the adsorption/activation of NO and H2O while further enhancing the NH3 selectivity from 76.9 % to 92.6 % (at 270 degrees C). Meanwhile, Fe sites act as electron acceptors to separate photoexcited carriers, synergizing with thermocatalytic high-temperature activation to overcome single-mode limitations. This study provides valuable ideas for photo-assisted thermocatalytic technology for ammonia synthesis under mild conditions.
Keyword ：
Electron transfer Electron transfer NO ammonia synthesis NO ammonia synthesis Oxygen vacancies Oxygen vacancies Pd-O-Fe interface Pd-O-Fe interface Photo-assisted thermocatalytic Photo-assisted thermocatalytic
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| GB/T 7714 | Li, Aoqiang , Li, Jianfei , Liang, Chaowei et al. Concurrent incorporation of Fe doping and construction of Pd-O-Fe interface for Pd/CeO2 photo-assisted thermocatalytic NO reduction into ammonia [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
| MLA | Li, Aoqiang et al. "Concurrent incorporation of Fe doping and construction of Pd-O-Fe interface for Pd/CeO2 photo-assisted thermocatalytic NO reduction into ammonia" . | CHEMICAL ENGINEERING JOURNAL 522 (2025) . |
| APA | Li, Aoqiang , Li, Jianfei , Liang, Chaowei , Meng, Xiangyu , Fu, Xianzhi , Dai, Wenxin . Concurrent incorporation of Fe doping and construction of Pd-O-Fe interface for Pd/CeO2 photo-assisted thermocatalytic NO reduction into ammonia . | CHEMICAL ENGINEERING JOURNAL , 2025 , 522 . |
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Solar-driven one-step disproportionation overall nitrogen fixation (ONF) for synchronously synthesizing ammonia and nitrate presents a promising alternative to conventional Haber-Bosch and Ostwald processes, but suffers from ultra-low efficiency. Single atoms (SAs) featured by maximized atomic utilization exhibit superb catalytic activity, while the definite electronic configurations confine SAs to function solely as reduction or oxidation sites, limiting the possibility for both reduction and oxidation reactions. Herein, an efficient approach is presented for ammonia and nitrate co-synthesis by introducing Fe SAs and alternating piezoelectric field into a defective piezoelectric BaTiO3 (OvBTO-Fe), enabling the formation spatially-separated redox regions and dynamic bidirectional switching of Fe spin states. At positive and negative polarization ends, Fe spin state transitions to high and low spin states through d-electrons relocation, respectively, thermodynamically and kinetically facilitate nitrogen reduction and oxidation reactions. Thus, OvBTO-Fe exhibits unprecedented piezo-photocatalytic ONF activity, achieving a record solar-to-chemical conversion efficiency of 0.82% and total energy-to-chemical conversion efficiency of 0.53%. This work proposes a methodology for dynamic multi-directional manipulation of spin states and overall catalytic synthesis reaction.
Keyword ：
nitrogen oxidation nitrogen oxidation nitrogen reduction nitrogen reduction piezo-photocatalysis piezo-photocatalysis single atom single atom spin state regulation spin state regulation
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| GB/T 7714 | Yuan, Jie , Chen, Fang , Feng, Wenhui et al. Dynamic Switching Spin State of Fe Single Atoms for Piezoelectric-Mediated Overall Nitrogen Fixation Photosynthesis [J]. | ADVANCED MATERIALS , 2025 , 37 (32) . |
| MLA | Yuan, Jie et al. "Dynamic Switching Spin State of Fe Single Atoms for Piezoelectric-Mediated Overall Nitrogen Fixation Photosynthesis" . | ADVANCED MATERIALS 37 . 32 (2025) . |
| APA | Yuan, Jie , Chen, Fang , Feng, Wenhui , Xiao, Jianyu , Wang, Liang , Luo, Songyu et al. Dynamic Switching Spin State of Fe Single Atoms for Piezoelectric-Mediated Overall Nitrogen Fixation Photosynthesis . | ADVANCED MATERIALS , 2025 , 37 (32) . |
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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 , 35 (25) . |
| MLA | Xiao, Zhen et al. "Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH" . | ADVANCED FUNCTIONAL MATERIALS 35 . 25 (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 , 35 (25) . |
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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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Two dimensional (2D) nanosheet photocatalysts have received intensive attention for various incomparable advantages. However, fabricating single-atom-thick photocatalyst nanosheets remains challenging. In this work, we developed monolayer nanosheets of Ti0.91O2 photocatalysts via the hydrazine assisted hydrothermal exfoliation of multilayer nanosheets. The hydrazine hydrate used for exfoliation can simultaneously serve as a sacrificial agent. Thepristine monolayer Ti0.91O2 photocatalysts achieved a hydrogen production rate of 6.22 mmol h-1 g-1 from water splitting, representing a fourfold enhancement over multilayer nanosheets. Upon loading Pt nanoparticles, the hydrogen production activity of Ti0.91O2 monolayer nanosheets increased to 13.28 mmol h-1 g-1. The monolayer nanosheets of Ti0.91O2 photocatalysts markedly enhanced the separation efficiency of photogenerated charge carriers. Furthermore, we demonstrate that the photogenerated electrons migrate to the edge of Ti0.91O2 monolayer nanosheets for the reduction reaction, while the photooxidation occurred on the surface of the nanosheets. This study provides valuable insights into the design of nanosheet photocatalysts.
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| GB/T 7714 | Qiu, Canyi , Xu, Mukun , Han, Shitong et al. Building monolayer Ti0.91O2 nanosheets to enhance hydrogen production for photocatalytic water splitting [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2025 , 15 (19) : 5827-5836 . |
| MLA | Qiu, Canyi et al. "Building monolayer Ti0.91O2 nanosheets to enhance hydrogen production for photocatalytic water splitting" . | CATALYSIS SCIENCE & TECHNOLOGY 15 . 19 (2025) : 5827-5836 . |
| APA | Qiu, Canyi , Xu, Mukun , Han, Shitong , Guo, Liuhan , Zhao, Hua , Shen, Jinni et al. Building monolayer Ti0.91O2 nanosheets to enhance hydrogen production for photocatalytic water splitting . | CATALYSIS SCIENCE & TECHNOLOGY , 2025 , 15 (19) , 5827-5836 . |
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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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Photocatalytic CO2 reduction offers a promising solution to both the energy crisis and environmental issues. However, existing photocatalysts for simulating photosynthesis at ambient temperature exhibit limited conversion efficiency. In this study, we leveraged the photothermal effect of MnO2 to significantly increase the surface temperature of the catalyst under full-spectrum irradiation, thereby markedly enhancing CO2 conversion efficiency. Photocatalytic performance evaluations and characterization results revealed that the temperature elevation accelerated the generation and transfer of photogenerated electrons. Furthermore, Cd single atoms (Cd SAs) were successfully incorporated onto the MnO2 surface through in-situ redox reaction. Various characterizations and first-principles calculations demonstrated that the incorporation of Cd SAs in Cd-MnO2 created effective atomic-level site for water adsorption and dissociation, providing abundant *H species for CO2 reduction. Cd SAs also modulate the local electronic environment, facilitating CO2 adsorption at adjacent Mn sites and lowering the energy barrier for *COOH formation. Moreover, the spin polarization induced by Cd SAs suppresses photogenerated charge recombination while promoting cyclic regeneration of active Mn sites. Furthermore, the weak adsorption of CO on the catalyst hinders its hydrogenation to CH4, achieving exceptional CO selectivity (98 %) with a production rate of 318.2 mu mol center dot g-1 center dot h-1. These advantages enhanced thermally-assisted photocatalytic performance, providing valuable insights for improving the efficiency of photocatalytic CO2 reduction.
Keyword ：
Cadmium single atoms Cadmium single atoms CO 2 Reduction CO 2 Reduction MnO2 MnO2 Photogenerated charge separation Photogenerated charge separation Thermally-assisted photocatalysis Thermally-assisted photocatalysis
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| GB/T 7714 | Ni, Wenkang , Sun, Xu , Zhang, Xiaoyan et al. Cadmium single atoms enhance full-spectrum solar photothermal-driven photocatalytic CO2 reduction in H2O vapor [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 369 . |
| MLA | Ni, Wenkang et al. "Cadmium single atoms enhance full-spectrum solar photothermal-driven photocatalytic CO2 reduction in H2O vapor" . | SEPARATION AND PURIFICATION TECHNOLOGY 369 (2025) . |
| APA | Ni, Wenkang , Sun, Xu , Zhang, Xiaoyan , Zhang, Zizhong , Wang, Ke , Dai, Wenxin et al. Cadmium single atoms enhance full-spectrum solar photothermal-driven photocatalytic CO2 reduction in H2O vapor . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 369 . |
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