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学者姓名：戴文新
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Abstract ：
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 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 methane conversion into liquid oxygenates using O-2 oxidants provides a promising approach for high-value chemicals. The generation of reactive oxygen species and their reaction pathway are key to determine the oxygenate selectivity. Here, an interstitial Zn-i defect ZnO (ZnO(Zn-i)) is developed through thermal decomposition of the ZnO2 precursor. Zn-i favors the O-2 adsorption at a terminal adsorption configuration and induces effectively the conversion O-2 into the desired center dot OOH instead of center dot OH for improving the yield and selectivity of oxygenates. For comparison, O-2 adsorbed in a lateral configuration tends to be converted into excessive center dot OH on the typical Au/ZnO. As a result, ZnO(Zn-i) shows the liquid oxygenates yield of 6080 mu mol g(-1) with 98.6% selectivity, which leads to 10 times lower than Au/ZnO for CO2 release of overoxidation. This work provides a pathway for O-2 adsorption and activation to regulate the photocatalytic CH4 oxidation conversion into liquid oxygenates.
Keyword ：
defects defects interstitial zinc interstitial zinc methane conversion methane conversion oxygen activation oxygen activation selectivity selectivity
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| GB/T 7714 | Xiao, Zhen , Wan, Zhenyu , Zhang, Jiangjie et al. Interstitial Zinc Defects Enriched ZnO Tuning O2 Adsorption and Conversion Pathway for Superior Photocatalytic CH4 Oxygenation [J]. | ACS CATALYSIS , 2024 . |
| MLA | Xiao, Zhen et al. "Interstitial Zinc Defects Enriched ZnO Tuning O2 Adsorption and Conversion Pathway for Superior Photocatalytic CH4 Oxygenation" . | ACS CATALYSIS (2024) . |
| APA | Xiao, Zhen , Wan, Zhenyu , Zhang, Jiangjie , Jiang, Jianing , Li, Dongmiao , Shen, Jinni et al. Interstitial Zinc Defects Enriched ZnO Tuning O2 Adsorption and Conversion Pathway for Superior Photocatalytic CH4 Oxygenation . | ACS CATALYSIS , 2024 . |
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Converting CO2 into hydrocarbons using solar energy enables the seamless integration of efficient solar energy utilization and carbon neutrality, presenting an efficacious solution to simultaneously tackle energy and environmental issues. However, challenges arise in controlling the selectivity of reduction products hinder its industrial application due to uncertainties in decisive factors. Given the complexity of the photocatalytic process, it is imperative to improve the understanding of the thermodynamic aspects (including consideration of both redox potential of photocatalysts and light absorption properties, activation of stable CO2 molecules, similarity in reduction potential of products) as well as kinetic obstacles (such as high adsorption potential, significant time disparity between charge separation and transfer, competition from side reactions). This Review offers a comprehensive analysis of the factors that govern product selectivity and explores effective strategies for enhancing catalytic performance based on recent advancements in photocatalytic CO2 reduction to diverse chemical compounds. These profound insights provide invaluable guidance for addressing challenges in practical applications of photocatalytic CO2 conversion.
Keyword ：
Activity Activity CO2 reduction CO2 reduction Photocatalysis Photocatalysis Reactionmechanism Reactionmechanism Selectivity Selectivity
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| GB/T 7714 | Wang, Shuowen , Wang, Jiashun , Wang, Ying et al. Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors [J]. | ACS CATALYSIS , 2024 , 14 (14) : 10760-10788 . |
| MLA | Wang, Shuowen et al. "Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors" . | ACS CATALYSIS 14 . 14 (2024) : 10760-10788 . |
| APA | Wang, Shuowen , Wang, Jiashun , Wang, Ying , Sui, Xiaoyu , Wu, Shuhong , Dai, Wenxin et al. Insight into the Selectivity-Determining Step of Various Photocatalytic CO2 Reduction Products by Inorganic Semiconductors . | ACS CATALYSIS , 2024 , 14 (14) , 10760-10788 . |
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Pollution in water environments hinders both social progress and economic development. Wastewater treatment and the sustainable use of water resources are important factors in solving this problem. In a previous study, the authors proposed a process that used photocatalytic film as a back-end treatment in a composite iron-carbon constructed wetland (WIC&PF) to restore a mildly eutrophic water body. This method has strong reoxygenation effects, and can efficiently remove pollutants; these are qualities that have not been mentioned in previous studies regarding constructed wetlands. In this study, the authors further investigated the effectiveness of this process by using a photocatalytic film as a front-end treatment for a composite iron-carbon constructed wetland (PF&WIC) to restore a mildly eutrophic water body. The results showed NH4+-N, TN, TP, COD, and chlorophyll a removal rates using PF&WIC of 79.1 +/- 6.6%, 76.8 +/- 6.5%, 77.0 +/- 5.4%, 77.3 +/- 7.2%, and 91.7 +/- 5.6%, respectively. The DO concentration of the water body increased compared with that of the effluent. The bacterial species and their abundance in the lake water also changed significantly, and photosynthetic autotrophic bacteria (Cyanobium PCC-6307) became the most dominant bacteria, and this played an important role in reoxygenating the water body. In comparing these results to those of our previous study, the removal of pollutants with PF&WIC was close to that with WIC&PF, but the reoxygenation effect of PF&WIC on the water body was significantly worse than that of WIC & PF; thus, WIC&PF is the more reasonable choice for treating eutrophic water bodies.
Keyword ：
constructed wetland constructed wetland photoautotrophic bacteria photoautotrophic bacteria photocatalytic film photocatalytic film reoxygenation reoxygenation sustainable utilization sustainable utilization water pollution water pollution
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| GB/T 7714 | Chen, Shihao , Ye, Ming , Chen, Nuo et al. Study of a New Photocatalytic Film Process Combined with a Constructed Wetland and an Analysis of Reoxygenation Pathways in a Water Body [J]. | SUSTAINABILITY , 2024 , 16 (8) . |
| MLA | Chen, Shihao et al. "Study of a New Photocatalytic Film Process Combined with a Constructed Wetland and an Analysis of Reoxygenation Pathways in a Water Body" . | SUSTAINABILITY 16 . 8 (2024) . |
| APA | Chen, Shihao , Ye, Ming , Chen, Nuo , Pan, Wenbin , Dai, Wenxin . Study of a New Photocatalytic Film Process Combined with a Constructed Wetland and an Analysis of Reoxygenation Pathways in a Water Body . | SUSTAINABILITY , 2024 , 16 (8) . |
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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 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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Membrane distillation technology, utilized for treating hypersaline wastewater from seawater desalination, often encounters challenges related to inorganic scaling, adversely affecting membrane performance. Herein, we introduce a innovative approach employing a sacrificial layer on the surface of Thin Film Composite (TFC) membranes to concurrently enhance inorganic scaling resistance and facilitate membrane reusability. The sacrificial layer (Fe3+-TA) consisted of tannic acid (TA) complexed with iron ions (Fe3+) and could be removed and regenerated in situ. The results demonstrated that the Fe3+-TA layer significantly improved the membrane's surface smoothness and densification, maintaining superior anti-scaling performance. The modified membrane exhibited remarkable durability, sustaining six reuse cycles with a flux recovery exceeding 97 % in gypsum scaling tests. Furthermore, the formation of new complexes during gypsum scaling tests confirmed the membrane's augmented scaling retardation capabilities. Thus, integrating of a sacrificial layer into TFC membranes presents a promising strategy for advancing membrane distillation processes in hypersaline wastewater treatment. © 2024 Elsevier B.V.
Keyword ：
Anti-scaling Anti-scaling Inorganic scaling Inorganic scaling Membrane distillation Membrane distillation Reuse Reuse Sacrificial protective layer Sacrificial protective layer
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| GB/T 7714 | Yan, Z. , Lin, S. , Chang, H. et al. Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation [J]. | Journal of Membrane Science , 2024 , 710 . |
| MLA | Yan, Z. et al. "Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation" . | Journal of Membrane Science 710 (2024) . |
| APA | Yan, Z. , Lin, S. , Chang, H. , Xu, J. , Dai, W. , Qu, D. et al. Functional of thin-film composite Janus membrane with sacrificial layer for inorganic scaling control in membrane distillation . | Journal of Membrane Science , 2024 , 710 . |
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The progressive transfer of photogenerated electrons between the catalyst components and reactants is of great significance for photocatalysis. Amorphous Pd (PdA) and oxygen vacancies (VOs) were simultaneously introduced in Pd-In2O3 exploiting hydrogen-induced amorphization effects; 0.6 wt% Pd-In2O3 exhibited a 4.5-fold increase in activity and a 3.2-fold higher selectivity toward CH3OH + CO (63.62 %) compared with In2O3. Multiple in situ techniques and theoretical calculations revealed that intercomponent electron transfer channels were established via various interface structures formed between PdA or crystalline Pd (PdC) and In2O3; PdA acted as electronic pump, facilitating the transfer and separation of photogenerated electrons, resulting in their subsequent enrichment on the surface of PdA. Simultaneously, PdA acted as electron-donating adsorption site for H2O, increasing the number of electrons received by H2O, further inhibiting the competitive adsorption of H2O and CO2 on VO sites, and promoting the hydrogen evolution reaction. Additionally, the electronic coupling between PdC and VOs could significantly decrease the electron-donating ability of VOs, reducing the number of electrons received by CO2, thus effectively regulating the degree of CO2 reduction. This study employs PdA/PdC and VOs to synergistic optimize the progressive transfer of photogenerated electrons, and presents a novel approach for elucidating the catalytic mechanism.
Keyword ：
Adsorption Behavior Adsorption Behavior Amorphous Pd Amorphous Pd CO 2 Photoreduction CO 2 Photoreduction Electron Transfer Electron Transfer Oxygen Vacancies Oxygen Vacancies
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| GB/T 7714 | Wang, Zhongming , Yuan, Hang , Chen, Siting et al. Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 492 . |
| MLA | Wang, Zhongming et al. "Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies" . | CHEMICAL ENGINEERING JOURNAL 492 (2024) . |
| APA | Wang, Zhongming , Yuan, Hang , Chen, Siting , Jia, Yong , Guo, Lina , Wang, Hong et al. Photoreduction of CO2 on Pd-In2O3: Synergistic optimization of progressive electron transfer via amorphous/crystalline Pd and oxygen vacancies . | CHEMICAL ENGINEERING JOURNAL , 2024 , 492 . |
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Solar-driven methanation of carbon dioxide (CO2) with water (H2O) has emerged as an important strategy for achieving both carbon neutrality and fuel production. The selective methanation of CO2 was often hindered by the sluggish kinetics and the multiple competition of other C1 byproducts. To overcome this bottleneck, we utilized a biomass synthesis method to synthesize SiC rods and then constructed a direct Z-scheme heterojunction Co3O4/SiC catalyst. The substantial difference in work functions between SiC and Co3O4 served as a significant source of the charge driving force, facilitating the conversion of CO2 to CH4. The high-valent cobalt Co(IV) in Co3O4 acts as an active species to promote efficient dissociation of water. This favorable condition greatly enhanced the likelihood of a high concentration of electrons and protons around a single site on the catalyst surface for CO2 methanation. DFT calculation showed that the energy barrier of CO2 hydrogenation was significantly reduced at the Co3O4/SiC heterojunction interface, which changed the reaction pathway and completely converted the product from CO to CH4. The optimum CH4 evolution rate of Co3O4/SiC samples was 21.3 μmol g-1 h-1 with 100% selectivity. This study has an important guiding significance for the selective regulation of CO2 to CH4 products in photocatalysis applications. © 2024 American Chemical Society.
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| GB/T 7714 | Lin, M. , Cai, Q. , Xiao, Z. et al. Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity [J]. | Inorganic Chemistry , 2024 , 63 (31) : 14591-14601 . |
| MLA | Lin, M. et al. "Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity" . | Inorganic Chemistry 63 . 31 (2024) : 14591-14601 . |
| APA | Lin, M. , Cai, Q. , Xiao, Z. , Chen, H. , Wang, B. , Qiu, C. et al. Cooperation of Strong Electric Field and H2O Dissociation on Co3O4-Decorated SiC Rods for Photodriven CO2 Methanation with 100% Selectivity . | Inorganic Chemistry , 2024 , 63 (31) , 14591-14601 . |
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