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学者姓名：沈锦妮
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Abstract ：
Solid solutions are garnering substantial attention in the realm of solar energy utilization due to their tunable electronic properties, encompassing band edge positions and charge-carrier mobilities. In this study, we designed and synthesized Co1-xZnxFe2xGa2-2xO4 (0<x <= 0.6) as a photocatalyst for CO2 conversion using H2O. Careful optical and photo/electrochemical characterizations unveiled that the relative content of CoGa2O4 and ZnFe2O4 not only substantially influences light absorption in the full solar spectrum but also modulates valence and conduction band positions. We thoroughly assessed the photocatalytic activity of Co1-xZnxFe2xGa2-2xO4 and found that when x=0.35, the solid-solution catalyst achieved a remarkable CO2 reduction rate to CH4 and CO (31.5 mu mol g(-1) h(-1)). Furthermore, this optimized solid-solution catalyst demonstrated impressive photostability. Characterization and DFT calculations revealed that the formation of a solid solution not only reduces the band gap and promotes the separation of electron-hole pairs to accelerate efficient CO2 photoreduction, but also the introduction of more FeO6 octahedral active sites in Co1-xZnxFe2xGa2-2xO4 solid solutions enhanced the effective photoreduction of CO2. This design results in high conversion efficiencies for producing solar fuels through CO2 reduction with H2O.
Keyword ：
Co1-xZnxFe2xGa2-2xO4 Co1-xZnxFe2xGa2-2xO4 CO2 conversion CO2 conversion molten salts molten salts photosynthesis photosynthesis Solid solution Solid solution
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| GB/T 7714 |
Wang, Qiang
,
Li, Li
,
Lu, Jiaxue
et al.
Construction of Co1-xZnxFe2xGa2-2xO4 (0 |
| MLA |
Wang, Qiang
et al.
"Construction of Co1-xZnxFe2xGa2-2xO4 (0 |
| APA |
Wang, Qiang
,
Li, Li
,
Lu, Jiaxue
,
Chai, Yao
,
Shen, Jinni
,
Liang, Jun
.
Construction of Co1-xZnxFe2xGa2-2xO4 (0 |
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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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Effective charge separation and migration pose a critical challenge in the field of solar-driven hydrogen production. In this work, a Z-scheme structured CuInS2/ZnIn2S4 heterojunction was successfully fabricated through a two-step hydrothermal synthesis method to significantly enhance the efficiency of solar-to-hydrogen energy conversion. Structural characterization revealed that the lattice-matched CuInS2/ZnIn2S4 heterojunction exhibits an enlarged interfacial contact area, which facilitates the transfer and separation of photogenerated charges. Microscopic analysis indicated that the CuInS2/ZnIn2S4 composite material has a tightly interwoven interface and a morphology resembling small sugar cubes. Photoelectrochemical spectroscopy analysis demonstrated that the heterojunction structure effectively enhances visible light absorption and charge separation efficiency, leading to an improvement in photocatalytic activity. Hydrogen production experimental data indicated that the CuInS2/ZnIn2S4 heterojunction photocatalyst prepared with a CuInS2 content of 20 wt% exhibits the highest hydrogen evolution rate, reaching 284.9 mu molg(-1)h(-1). Moreover, this photocatalyst maintains robust photocatalytic stability even after three consecutive usage cycles. This study demonstrated that the Z-scheme CuInS2/ZnIn2S4 heterojunction photocatalyst exhibits enhanced hydrogen evolution efficiency, offering an effective structural design for harnessing solar energy to obtain hydrogen fuel. Therefore, this heterojunction photocatalyst is a promising candidate for practical applications in solar hydrogen production.
Keyword ：
CuInS2/ZnIn2S4 photocatalyst CuInS2/ZnIn2S4 photocatalyst hydrogen evolution reaction hydrogen evolution reaction visible light performance visible light performance Z-scheme heterojunctions Z-scheme heterojunctions
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| GB/T 7714 | Li, Fuying , Liao, Boiyee , Shen, Jinni et al. Enhancing Photocatalytic Activities for Sustainable Hydrogen Evolution on Structurally Matched CuInS2/ZnIn2S4 Heterojunctions [J]. | MOLECULES , 2024 , 29 (11) . |
| MLA | Li, Fuying et al. "Enhancing Photocatalytic Activities for Sustainable Hydrogen Evolution on Structurally Matched CuInS2/ZnIn2S4 Heterojunctions" . | MOLECULES 29 . 11 (2024) . |
| APA | Li, Fuying , Liao, Boiyee , Shen, Jinni , Ke, Junni , Zhang, Rongxin , Wang, Yueqi et al. Enhancing Photocatalytic Activities for Sustainable Hydrogen Evolution on Structurally Matched CuInS2/ZnIn2S4 Heterojunctions . | MOLECULES , 2024 , 29 (11) . |
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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 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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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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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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Photocatalytic conversion of CO2 into valued chemicals has evoked broad interest. However, the photocatalytic efficiency is limited by the adsorption and activation capability of the catalyst surface for CO2. Here, isomor-phically Sn (IV) doped BiOBr is achieved through a facile chemical method. The as-prepared Sn-doped BiOBr demonstrates the enhanced performance of photocatalytic CO2 reduction into CO. Thereinto, the 4Sn-BiOBr sample shows the best activity with the CO yield of 165.6 mu mol center dot g- 1 center dot h-1, which is 7.8 times higher than that of pristine BiOBr. Sn ions and oxygen vacancies (OVs) are shown to be simultaneously introduced into the crystal lattice of BiOBr. As a result, surface frustrated Lewis acidic sites and Lewis basic sites of BiOBr are constructed and the activation capability for CO2 is improved obviously. This work presents the feasible tunability of catalytic active sites for catalyst at atom-scale, and offers fundamental insights for understanding of the mechanism of photocatalytic CO2 reduction.
Keyword ：
BiOBr BiOBr CO2 photoreduction CO2 photoreduction Photocatalytic mechanism Photocatalytic mechanism Sn isomorphous substitution Sn isomorphous substitution Surface frustrated Lewis acid-base pairs Surface frustrated Lewis acid-base pairs
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| GB/T 7714 | Hao, Jie , Zhang, Yanfeng , Zhang, Lei et al. Restructuring surface frustrated Lewis acid-base pairs of BiOBr through isomorphous Sn doping for boosting photocatalytic CO2 reduction [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 464 . |
| MLA | Hao, Jie et al. "Restructuring surface frustrated Lewis acid-base pairs of BiOBr through isomorphous Sn doping for boosting photocatalytic CO2 reduction" . | CHEMICAL ENGINEERING JOURNAL 464 (2023) . |
| APA | Hao, Jie , Zhang, Yanfeng , Zhang, Lei , Shen, Jinni , Meng, Lingpeng , Wang, Xuxu . Restructuring surface frustrated Lewis acid-base pairs of BiOBr through isomorphous Sn doping for boosting photocatalytic CO2 reduction . | CHEMICAL ENGINEERING JOURNAL , 2023 , 464 . |
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Photocatalytic converting CO2 into C-2 products is highly desirable but is extremely sensitive to catalyst structure. In this work, Ti-H species and oxygen vacancies are simultaneously integrated on hydrogenated SrTiO3 surface by thermally treating with NaBH4, which promotes the activation of CO2 into HCOO- and CO* intermediates. The proximity of oxygen vacancies and Ti-H species contributes to the C-C coupling of intermediates into acetylene (C2H2) products. To the best of our knowledge, this is the first example for the photocatalytic CO2 reduction into C2H2 main products. The optimal hydrogenated SrTiO3 has the C2H2 yield of 39.0 mu mol center dot g(-1) with a 76.0 % selectivity among C-2 products. Therefore, this work provides an approach of designing the adjacent active sites for photocatalytic CO2 conversion into C2+ products.
Keyword ：
C-C coupling C-C coupling CO2 reduction CO2 reduction Defect sites Defect sites Photocatalysis Photocatalysis Ti-H species Ti-H species
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| GB/T 7714 | Xu, Haiying , Wang, Zhaoliang , Liao, Hehua et al. Proximity of defects and Ti-H on hydrogenated SrTiO3 mediated photocatalytic reduction of CO2 to C2H2 [J]. | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 336 . |
| MLA | Xu, Haiying et al. "Proximity of defects and Ti-H on hydrogenated SrTiO3 mediated photocatalytic reduction of CO2 to C2H2" . | APPLIED CATALYSIS B-ENVIRONMENTAL 336 (2023) . |
| APA | Xu, Haiying , Wang, Zhaoliang , Liao, Hehua , Li, Dongmiao , Shen, Jinni , Long, Jinlin et al. Proximity of defects and Ti-H on hydrogenated SrTiO3 mediated photocatalytic reduction of CO2 to C2H2 . | APPLIED CATALYSIS B-ENVIRONMENTAL , 2023 , 336 . |
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Solar light-driven overall water splitting for hydrogen production is an ideal solution to climate warming and energy shortage issues. Obtaining a highly efficient and stable photocatalyst remains a major challenge at present. Herein, NixP/gamma-Ga2O3 nanosheets, which were synthesized from NiCl2, NaH2PO2, and home-made gamma-Ga2O3 nanosheets by the photodeposition method under 254 UV irradiation for 30 min, are found as a highly active and durable photocatalyst for pure water splitting into H2 and O2 without a sacrificial reagent. The H2 production rate is as high as 5.5 mmol center dot g-1 center dot h-1 under 125 W high-pressure mercury lamp irradiation, which is 3.4 and 2.5 times higher than that on the pristine gamma-Ga2O3 nanosheets and Pt/gamma-Ga2O3 nanosheets, respectively, and is 2.0 times higher than that on the 0.5 wt % Ni2P/gamma-Ga2O3 reported previously. However, the O2 evolution rate is much less than the H2 evolution rate in the initial reaction stage. On prolonging the irradiation time, H2 evolution declines, while O2 evolution increases until it reaches its stoichiometric value corresponding to H2. The reason for the photocatalytic behavior of NixP/gamma-Ga2O3 is studied and the corresponding mechanism is suggested. The absent or low oxygen evolution in the initial reaction stage is because the dioxygen generated from water oxidation by the photogenerated holes is wholly or partially captured by the surface oxygen vacancies to form the surface peroxide bonds (-O-O-). Once the oxygen vacancies are eliminated by the photogenerated O2, the overall water splitting reaction would reach the steady state. Thereafter, H2 production decreases from 5.5 to 2.0 mmol center dot g-1 center dot h-1, but the O2 evolution gradually approaches the corresponding stoichiometric value, especially for the photocatalyst treated with H2O2 for 24 h.
Keyword ：
NixP NixP overall water splitting overall water splitting photocatalyst photocatalyst reaction mechanism reaction mechanism
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| GB/T 7714 | Shen, Jinni , Liu, Xu , Zhong, Yuhua et al. Photocatalytic Overall Water Splitting Reaction Feature on Photodeposited NiXP/?-Ga2O3 Nanosheets [J]. | ACS APPLIED ENERGY MATERIALS , 2023 , 6 (8) : 4317-4326 . |
| MLA | Shen, Jinni et al. "Photocatalytic Overall Water Splitting Reaction Feature on Photodeposited NiXP/?-Ga2O3 Nanosheets" . | ACS APPLIED ENERGY MATERIALS 6 . 8 (2023) : 4317-4326 . |
| APA | Shen, Jinni , Liu, Xu , Zhong, Yuhua , Qiu, Chengwei , Xu, Huihui , He, Hongsheng et al. Photocatalytic Overall Water Splitting Reaction Feature on Photodeposited NiXP/?-Ga2O3 Nanosheets . | ACS APPLIED ENERGY MATERIALS , 2023 , 6 (8) , 4317-4326 . |
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