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学者姓名：王绪绪
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Abstract ：
Construction of S-scheme heterojunction for photocatalytic conversion of CO2 into carbon-neutral fuels under sunlight is of paramount value for the sustainable development of energy. However, few reports are concerned the local structure and electronic structure of semiconductor heterojunction, which are importance of understanding the effect of heterojunction structure on the photocatalytic property. In this work, hierarchical alpha-Fe2O3/ g-C3N4 S-scheme heterojunctions were manufactured via an in situ self-assembly strategy for the efficient reduction of CO2. The generation rate of main product CO for optimal alpha-Fe2O3/g-C3N4 heterojunction is up to 215.8 mu mol g-1 h-1, with selectivity of 93.3 %, which is 17.5 and 6.1 times higher than those of pristine Fe2O3 and g-C3N4, respectively. The local structure and electronic structure for alpha-Fe2O3/g-C3N4 heterojunction are probed by hard X-Ray Absorption Fine Structure (XAFS) and soft X-Ray Absorption Spectroscopy (XAS), as well as density-functional theory (DFT) calculations. It is found that the Fe(d)-N(p) bond formed in alpha-Fe2O3/g-C3N4 heterojunction precisely connects the conduction band (CB) of Fe2O3 and the valence band (VB) of g-C3N4, which minimizes the charge transfer distance and facilitates CO2 photoreduction activity. This work provides important information for understanding the influence of interface local and electronic structure on the performance of photo-catalytic reduction of CO2 at the atomic level.
Keyword ：
alpha-Fe 2 O 3 /g-C 3 N 4 alpha-Fe 2 O 3 /g-C 3 N 4 CO 2 photoreduction CO 2 photoreduction Interface Interface Local structure Local structure S -scheme S -scheme
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| GB/T 7714 | Qin, Jianyu , Zhao, Mengyue , Zhang, Yanfeng et al. Probing local structure and electronic structure of α-Fe2O3/g-C3N4 S-scheme heterojunctions for boosting CO2 photoreduction [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 685 : 1109-1121 . |
| MLA | Qin, Jianyu et al. "Probing local structure and electronic structure of α-Fe2O3/g-C3N4 S-scheme heterojunctions for boosting CO2 photoreduction" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 685 (2025) : 1109-1121 . |
| APA | Qin, Jianyu , Zhao, Mengyue , Zhang, Yanfeng , Shen, Jinni , Wang, Xuxu . Probing local structure and electronic structure of α-Fe2O3/g-C3N4 S-scheme heterojunctions for boosting CO2 photoreduction . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 685 , 1109-1121 . |
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Photocatalytic water splitting on metal oxides often faces oxygen evolution inefficiency, reflecting the complex interplay of its two half-reactions. Strategies like heterojunctions, cocatalyst loading, or noble metal nano- particles addition have been explored to address this. Using gamma- Ga 2 O 3 nanosheets as a model, we uncovered the formation of-O-O- species as the key barrier to stoichiometric splitting. To tackle this, a strategy was devised, Sr-doping to inhibit surface peroxidation. The resultant Sr-doped gamma- Ga 2 O 3 (Sr-Ga2O3) significantly improved activity and stability, achieving balanced H2 and O2 production under 125 W mercury lamp light. Upon further enhancement with Rh/Cr2O3 cocatalyst via photoreduction, the Sr-Ga2O3/(Rh/Cr2O3) composite demonstrated a remarkable 173.3 mu mol & sdot;h-1 H2 and 86.7 mu mol & sdot;h-1 O2 evolution rate, 8.0 times higher than gamma- Ga 2 O 3 alone, with a 34.1 % quantum efficiency under 260 nm light. This represents a record performance for Ga2O3-based photo- catalytic water splitting. Mechanistically, Sr doping alters surface chemistry to favor direct oxygen release. Our study elucidates molecular-level insights into non-stoichiometric splitting mechanisms and offers a potent strategy to boost metal oxide photocatalysts' water-splitting efficiency.
Keyword ：
Photocatalytic stoichiometric water splitting Photocatalytic stoichiometric water splitting Sr-doped Sr-doped
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| GB/T 7714 | Shen, Jinni , Zhong, Yuhua , Lin, Jianhan et al. Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution [J]. | JOURNAL OF CATALYSIS , 2025 , 443 . |
| MLA | Shen, Jinni et al. "Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution" . | JOURNAL OF CATALYSIS 443 (2025) . |
| APA | Shen, Jinni , Zhong, Yuhua , Lin, Jianhan , Li, Haifeng , Qiu, Chengwei , Liu, Xu et al. Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution . | JOURNAL OF CATALYSIS , 2025 , 443 . |
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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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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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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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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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Direct synthesis of urea from CO2, N-2, and H2O through photocatalysis stands out as an effective solution to mitigate the over-release of CO2 and alleviate the high costs associated with nitrogen fertilizer production. The 20% CdS@Bi2WO6 sample exhibits optimal activity under visible light, achieving a urea yield of 10.0 mu molg(-1)h(-1). The photocatalytic efficacy of this composite is attributed to its S-type heterojunction, which can significantly enhance the redox capacity and the efficiency of photogenerated charge separation compared to individual semiconductor components. CdS appears to be responsible for the photocatalytic reduction of N-2 and urea synthesis, while Bi2WO6 is involved in the oxidation of H2O to form O-2 and H+. It is suggested that urea is synthesized on the surface of CdS through two mechanisms: (I) the reaction between the activated intermediates of CO2 and N-2 (mainly) and (II) the reaction of the in situ formed NH3 with the feed CO2.
Keyword ：
CdS@Bi2WO6 CdS@Bi2WO6 nitrogen nitrogen photocatalysis photocatalysis S-type heterojunction S-type heterojunction urea urea
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| GB/T 7714 | Wang, Yingshu , Liu, Yanan , Gan, Jiasi et al. Visible-Light Photocatalytic CO2-N2-H2O to Urea with CdS@Bi2WO6 [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (39) : 14505-14513 . |
| MLA | Wang, Yingshu et al. "Visible-Light Photocatalytic CO2-N2-H2O to Urea with CdS@Bi2WO6" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 12 . 39 (2024) : 14505-14513 . |
| APA | Wang, Yingshu , Liu, Yanan , Gan, Jiasi , Hong, Lu , Shen, Jinni , Zhang, Zizhong et al. Visible-Light Photocatalytic CO2-N2-H2O to Urea with CdS@Bi2WO6 . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2024 , 12 (39) , 14505-14513 . |
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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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The serious combination of abundant electrons/holes in bulk primarily hinders the efficiency in the photocatalytic reaction. It is crucial to control the spatial charge dynamics through delicately designing the crystal configuration of photocatalyst. In this work, a modified tungsten trioxide nanosheet colloid (M-WO3) was synthesized by an ion exchange method. Compared to pristine WO3 (P-WO3), the crystal lattice vibration frequency of M-WO3 increases from 2.8 meV to 4.3 meV, which effectively prohibits electron-phonon coupling and powerfully accelerates the separation and transfer of photoinduced charge carriers. Irradiated by visible-light, M-WO3 shows much higher photocatalytic bacterial inactivation performance than P-WO3. In addition, this regulation method increases the surface charges of the WO3 colloid to improve its stability, which endows this colloid photocatalyst with broad prospects in practical photocatalytic antibacterial applications. This work offers guidance to construct efficiently separated photoinduced electron/hole pairs of the colloid photocatalyst by designing its crystal structure.
Keyword ：
Colloid photocatalyst Colloid photocatalyst Colloid stability Colloid stability Crystal lattice vibration frequency Crystal lattice vibration frequency Photocatalytic disinfection Photocatalytic disinfection WO(6)octahedra distortion WO(6)octahedra distortion
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| GB/T 7714 | Qiu, Chengwei , Liu, Zhihua , Rao, Qin et al. Prohibiting the electron-phonon coupling effect in tungsten trioxide nanosheet colloid with enhanced photocatalytic antibacterial capacity [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 678 : 1135-1147 . |
| MLA | Qiu, Chengwei et al. "Prohibiting the electron-phonon coupling effect in tungsten trioxide nanosheet colloid with enhanced photocatalytic antibacterial capacity" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 678 (2024) : 1135-1147 . |
| APA | Qiu, Chengwei , Liu, Zhihua , Rao, Qin , Yang, Hui , He, Yuxin , Li, Dongmiao et al. Prohibiting the electron-phonon coupling effect in tungsten trioxide nanosheet colloid with enhanced photocatalytic antibacterial capacity . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2024 , 678 , 1135-1147 . |
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