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学者姓名:戴文新
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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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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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Humic acid (HA), a widely prevalent natural organic matter in aquatic environments, poses serious health risks due to its potential to form carcinogenic by-products during water treatment. While the photo-Fenton process can be employed for HA degradation, its effectiveness is often hindered by the poor catalytic performance of conventional catalysts. In this study, Co3O4 was modified with nitrogen-doped carbon quantum dots (NCDs) and immobilized on a PVDF membrane. Compared with Co3O4/PVDF, Co3O4/NCDs/PVDF system achieved 85.1 % HA removal and 66 % mineralization within 60 min through photocatalytic peroxymonosulfate (PMS) activation as well as showed excellent stability in cycle experiments. The incorporation of NCDs enhanced the synergistic effect between light and PMS, improved light absorption due to the narrowed bandgap of Co3O4/NCDs/PVDF, and played a significant role in generating the primary reactive species, 1O2. Additionally, Co3O4/NCDs/PVDF effectively controlled Co ions leaching. Finally, the degradation intermediates were identified, and the degradation pathways were proposed. The photo-Fenton degradation of HA preferentially broke unsaturated bonds and degraded aromatic ring compounds. The Co3O4/NCDs/PVDF photo-Fenton catalytic system serves as an effective approach for boosting the efficiency of photo-Fenton degradation.
Keyword :
Carbon quantum dots Carbon quantum dots Humic acid Humic acid Peroxymonosulfate activation Peroxymonosulfate activation Photocatalysis Photocatalysis
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GB/T 7714 | Yan, Zhongsen , Li, Binbin , Liu, Guohui et al. Enhanced degradation of humic acid by Co3O4/NCDs/PVDF photo-Fenton catalytic system [J]. | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION , 2025 , 198 . |
MLA | Yan, Zhongsen et al. "Enhanced degradation of humic acid by Co3O4/NCDs/PVDF photo-Fenton catalytic system" . | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION 198 (2025) . |
APA | Yan, Zhongsen , Li, Binbin , Liu, Guohui , Lu, Zhenyu , Chang, Haiqing , Jin, Juxiang et al. Enhanced degradation of humic acid by Co3O4/NCDs/PVDF photo-Fenton catalytic system . | PROCESS SAFETY AND ENVIRONMENTAL PROTECTION , 2025 , 198 . |
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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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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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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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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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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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Heterojunction engineering is a powerful approach for improving the separation efficiency of photogenerated charge carriers. In this study, ultrathin 2D/2D CeVO4/WO3 center dot H2O heterojunction nanosheets are synthesized via electrostatic self-assembly of ultrathin CeVO4 (similar to 1.3 nm) and WO3 center dot H2O (similar to 2.4 nm) nanosheets for greatly enhancing photocatalytic CO2 reduction and H2O oxidation performance. The 2D heterojunction nanosheets process a Z-scheme charge transfer pathway to effectively promote charge separation efficiency and superior redox capabilities. Concurrently, the ultrathin heterojunction configuration substantially reduces the migration distance of charge carriers. These synergistic effects endow the CeVO4/WO3 center dot H2O composite with the marked CH4 and CO production rates of 8.4 mu mol center dot g(-1)center dot h(-1) and 38.5 mu mol center dot g(-1)center dot h(-1) under full-spectrum illumination. The CO generation rate of the ultrathin heterojunction surpasses pure WO3 center dot H2O by similar to 32 times and CeVO4 by similar to 18 times. This study also provides insights into the rational design of heterojunction nanosheet photocatalysts for CO2 reduction with H2O.
Keyword :
2D/2D heterojunctions 2D/2D heterojunctions CeVO4 CeVO4 Photocatalytic CO2 reduction Photocatalytic CO2 reduction Ultrathin nanosheets Ultrathin nanosheets WO3 center dot H2O WO3 center dot H2O
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GB/T 7714 | Fu, Chen , Li, Hongjiang , Jiang, Jianing et al. Building ultrathin nanosheet CeVO4/WO3•H2O Z-scheme heterojunction for boosting photocatalytic CO2 reduction [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 519 . |
MLA | Fu, Chen et al. "Building ultrathin nanosheet CeVO4/WO3•H2O Z-scheme heterojunction for boosting photocatalytic CO2 reduction" . | CHEMICAL ENGINEERING JOURNAL 519 (2025) . |
APA | Fu, Chen , Li, Hongjiang , Jiang, Jianing , Shen, Jinni , Long, Jinlin , Dai, Wenxin et al. Building ultrathin nanosheet CeVO4/WO3•H2O Z-scheme heterojunction for boosting photocatalytic CO2 reduction . | CHEMICAL ENGINEERING JOURNAL , 2025 , 519 . |
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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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