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学者姓名：王绪绪
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Abstract ：
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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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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Photocatalytic H2 evolution has been regarded as a promising technology to alleviate the energy crisis. Designing graphitic carbon nitride materials with a large surface area, short diffusion paths for electrons, and more exposed reactive sites are beneficial for hydrogen evolution. In this study, a facile method was proposed to dope P into a graphitic carbon nitride framework by calcining melamine with 2-aminoethylphosphonic acid. Meanwhile, PCN nanosheets (PCNSs) were obtained through a thermal exfoliation strategy. Under visible light, the PCNS sample displayed a hydrogen evolution rate of 700 μmol·g−1·h−1, which was 43.8-fold higher than that of pure g-C3N4. In addition, the PCNS photocatalyst also displayed good photostability for four consecutive cycles, with a total reaction time of 12 h. Its outstanding photocatalytic performance was attributed to the higher surface area exposing more reactive sites and the enlarged band edge for photoreduction potentials. This work provides a facile strategy to regulate catalytic structures, which may attract great research interest in the field of catalysis. © 2024 by the authors.
Keyword ：
graphitic carbon nitride graphitic carbon nitride hydrogen evolution hydrogen evolution P doped P doped thermal exfoliation thermal exfoliation
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| GB/T 7714 | Chen, L. , Zhang, L. , Xia, Y. et al. Thermal Exfoliation and Phosphorus Doping in Graphitic Carbon Nitride for Efficient Photocatalytic Hydrogen Production [J]. | Molecules , 2024 , 29 (15) . |
| MLA | Chen, L. et al. "Thermal Exfoliation and Phosphorus Doping in Graphitic Carbon Nitride for Efficient Photocatalytic Hydrogen Production" . | Molecules 29 . 15 (2024) . |
| APA | Chen, L. , Zhang, L. , Xia, Y. , Huang, R. , Liang, R. , Yan, G. et al. Thermal Exfoliation and Phosphorus Doping in Graphitic Carbon Nitride for Efficient Photocatalytic Hydrogen Production . | Molecules , 2024 , 29 (15) . |
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Efficient photocatalytic reduction of CO2 to high-calorific-value CH4, an ideal target product, is a blueprint for C-1 industry relevance and carbon neutrality, but it also faces great challenges. Herein, we demonstrate unprecedented hybrid SiC photocatalysts modified by Fe-based cocatalyst, which are prepared via a facile impregnation-reduction method, featuring an optimized local electronic structure. It exhibits a superior photocatalytic carbon-based products yield of 30.0 mu mol g(-1) h(-1) and achieves a record CH4 selectivity of up to 94.3%, which highlights the effectiveness of electron-rich Fe cocatalyst for boosting photocatalytic performance and selectivity. Specifically, the synergistic effects of directional migration of photogenerated electrons and strong pi-back bonding on low-valence Fe effectively strengthen the adsorption and activation of reactants and intermediates in the CO2 -> CH4 pathway. This study inspires an effective strategy for enhancing the multielectron reduction capacity of semiconductor photocatalysts with low-cost Fe instead of noble metals as cocatalysts.
Keyword ：
artificial synthesis of CH4 artificial synthesis of CH4 electronic structure optimization electronic structure optimization Fe species cocatalyst Fe species cocatalyst photocatalytic CO2 reduction photocatalytic CO2 reduction SiC SiC
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| GB/T 7714 | Lin, Qianying , Zhao, Jiwu , Zhang, Pu et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation [J]. | CARBON ENERGY , 2024 , 6 (1) . |
| MLA | Lin, Qianying et al. "Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation" . | CARBON ENERGY 6 . 1 (2024) . |
| APA | Lin, Qianying , Zhao, Jiwu , Zhang, Pu , Wang, Shuo , Wang, Ying , Zhang, Zizhong et al. Highly selective photocatalytic reduction of CO2 to CH4 on electron-rich Fe species cocatalyst under visible light irradiation . | CARBON ENERGY , 2024 , 6 (1) . |
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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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One-pot synthesis of urea [(NH2)(2)CO] from easily available small molecules, that is, N-2, CO2, and H2O, is an extremely attractive but very challenging reaction. 2D-CdS@3D-BiOBr composites with S-scheme heterojunctions are constructed via a facile hydrothermal technique followed by a self-assembly method and shown to be an excellent photocatalyst enabling the reduction of N-2 and CO2 with H2O to (NH2)(2)CO under visible light. The optimal 40%2D-CdS@3D-BiOBr sample shows up to 15 mu mol.g(-1).h(-1) total yield of NH3 and (NH2)(2)CO, of which (NH2)(2)CO accounts for 54%. The apparent quantum efficiency (AQE) is 3.93% for urea production. On the photocatalyst, urea is speculated to form by two possible chemical routes. One is direct photocatalytic synthesis. Both N-2 and CO2 molecules are activated by the Cd2+ ion of 2D-CdS and the oxygen defect of 3D-BiOBr at the edges of the heterojunction interface of 2D-CdS/3D-BiOBr, respectively. *HNCONH* is the key intermediate of the formation of (NH2)(2)CO molecules. The other is indirect synthesis by photocatalysis and then thermocatalysis. N-2 is reduced into NH3 and CO2 is reduced into CO on 2D-CdS by the photogenerated electrons and protons, and then the formed NH3 reacts with the reactant CO2 or the product CO to form (NH2)(2)CO by thermocatalysis on 2D-CdS. The former is dominant for urea synthesis. The work confirms that urea could be synthesized photocatalytically from cheap N-2, CO2, and H2O under visible light. A composite heterojunction semiconductor could be a prospective photocatalyst appropriate for the complex reaction.
Keyword ：
carbon dioxide carbon dioxide CdS@BiOBr composite CdS@BiOBr composite nitrogen nitrogen photocatalysis photocatalysis urea synthesis urea synthesis
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| GB/T 7714 | Wang, Yingshu , Wang, Shuyue , Gan, Jiasi et al. Photocatalytic Coreduction of N-2 and CO2 with H2O to (NH2)(2)CO on 2D-CdS/3D-BiOBr [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2023 , 11 (5) : 1962-1973 . |
| MLA | Wang, Yingshu et al. "Photocatalytic Coreduction of N-2 and CO2 with H2O to (NH2)(2)CO on 2D-CdS/3D-BiOBr" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 11 . 5 (2023) : 1962-1973 . |
| APA | Wang, Yingshu , Wang, Shuyue , Gan, Jiasi , Shen, Jinni , Zhang, Zizhong , Zheng, Huidong et al. Photocatalytic Coreduction of N-2 and CO2 with H2O to (NH2)(2)CO on 2D-CdS/3D-BiOBr . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2023 , 11 (5) , 1962-1973 . |
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New surface coordination photocatalytic systems that are inspired by natural photosynthesis have significant potential to boost fuel denitrification. Despite this, the direct synthesis of efficient surface coordination photocatalysts remains a major challenge. Herein, it is verified that a coordination photocatalyst can be constructed by coupling Pd and CTAB-modified ZnIn2S4 semiconductors. The optimized Pd/ZnIn2S4 showed a superior degradation rate of 81% for fuel denitrification within 240 min, which was 2.25 times higher than that of ZnIn2S4. From the in situ FTIR and XPS spectra of 1% Pd/ZnIn2S4 before and after pyridine adsorption, we find that pyridine can be selectively adsorbed and form Zn center dot center dot center dot C-N or In center dot center dot center dot C-N on the surface of Pd/ZnIn2S4. Meanwhile, the superior electrical conductivity of Pd can be combined with ZnIn2S4 to promote photocatalytic denitrification. This work also explains the surface/interface coordination effect of metal/nanosheets at the molecular level, playing an important role in photocatalytic fuel denitrification.
Keyword ：
denitrification denitrification photocatalysis photocatalysis pyridine pyridine surface coordination surface coordination ZnIn2S4 ZnIn2S4
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| GB/T 7714 | Wang, Deling , Zhan, Erda , Wang, Shihui et al. Surface Coordination of Pd/ZnIn2S4 toward Enhanced Photocatalytic Activity for Pyridine Denitrification [J]. | MOLECULES , 2023 , 28 (1) . |
| MLA | Wang, Deling et al. "Surface Coordination of Pd/ZnIn2S4 toward Enhanced Photocatalytic Activity for Pyridine Denitrification" . | MOLECULES 28 . 1 (2023) . |
| APA | Wang, Deling , Zhan, Erda , Wang, Shihui , Liu, Xiyao , Yan, Guiyang , Chen, Lu et al. Surface Coordination of Pd/ZnIn2S4 toward Enhanced Photocatalytic Activity for Pyridine Denitrification . | MOLECULES , 2023 , 28 (1) . |
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Metal-decorated oxide semiconductors are overwhelming photocatalysts for nonoxidative coupling of methane (NOCM). However, the overall NOCM mechanism remains an unopened black box, which hinders the design of high-performance catalysts. Herein, we systematically studied a series of noble metal (Ag, Au, Pt, Pd, Cu, and Ni)-decorated oxides (NaTaO3, CaTiO3, LiNbO3, and TiO2) for NOCM. We proposed that the active sites for H abstraction and C-C coupling of CH4 are spatially separated. Specifically, NaTaO3 only completes the initial H abstraction of CH4 activation, while metal nanoparticles are responsible for the final C-C coupling. Noble metals dominate NOCM by significantly decreasing the energy barrier of CH4 dissociation and promoting C-C coupling. Among various metals, Ag is preferential for the weak adsorption of center dot CH3 intermediates and subsequent metal-induced CC coupling. This contributes to Ag/NaTaO3 the highest C2H(6) yield of 194 mu mol g-1 h(-1) and stoichiometric H-2 with 11.2% quantum efficiency. This work provides a molecular-level insight into the CH4 coupling mechanism on metal-decorated photocatalysts.
Keyword ：
C C C coupling C coupling H activation H activation mechanism mechanism methane methane photocatalytic photocatalytic
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| GB/T 7714 | Zhang, Jiangjie , Shen, Jinni , Li, Dongmiao et al. Efficiently Light-Driven Nonoxidative Coupling of Methane on Ag/ NaTaO3: A Case for Molecular-Level Understanding of the Coupling Mechanism [J]. | ACS CATALYSIS , 2023 , 13 (3) : 2094-2105 . |
| MLA | Zhang, Jiangjie et al. "Efficiently Light-Driven Nonoxidative Coupling of Methane on Ag/ NaTaO3: A Case for Molecular-Level Understanding of the Coupling Mechanism" . | ACS CATALYSIS 13 . 3 (2023) : 2094-2105 . |
| APA | Zhang, Jiangjie , Shen, Jinni , Li, Dongmiao , Long, Jinlin , Gao, Xiaochen , Feng, Wenhui et al. Efficiently Light-Driven Nonoxidative Coupling of Methane on Ag/ NaTaO3: A Case for Molecular-Level Understanding of the Coupling Mechanism . | ACS CATALYSIS , 2023 , 13 (3) , 2094-2105 . |
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Cu2O is one of the most promising photocatalysts for visible light driven CO2 conversion, but its practical application in artificial photosynthesis is challenged to severe photocorrosion. Herein, a Cu2O/LaTiO2N composite is successfully synthesized by loading Cu2O on LaTiO2N through an ascorbic acid reduction method, which significantly improves the stability and activity of Cu2O for visible light driven photocat-alytic CO2 conversion, and shows higher photocatalytic performance than most Cu2O-based photocata-lysts reported. The superior photocatalytic performance is attributed to the formation of type-II heterojunction between Cu2O and LaTiO2N, which facilitates the separation and transfer of photogener-ated electrons and holes. This work provides an effective strategy for the construction of stable and effi-cient Cu2O-based photocatalysts. (c) 2022 Elsevier Inc. All rights reserved.
Keyword ：
Activity Activity Cu2O Cu2O LaTiO2N LaTiO2N PhotocatalyticCO2 reduction PhotocatalyticCO2 reduction Stability Stability
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| GB/T 7714 | Lin, Lichao , Lin, Peiling , Song, Jia et al. Boosting the photocatalytic activity and stability of Cu2O for CO2 conversion [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 630 : 352-362 . |
| MLA | Lin, Lichao et al. "Boosting the photocatalytic activity and stability of Cu2O for CO2 conversion" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 630 (2023) : 352-362 . |
| APA | Lin, Lichao , Lin, Peiling , Song, Jia , Zhang, Zizhong , Wang, Xuxu , Su, Wenyue . Boosting the photocatalytic activity and stability of Cu2O for CO2 conversion . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2023 , 630 , 352-362 . |
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