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学者姓名：沈锦妮
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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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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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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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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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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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Low-mass interfacial contacts and poor charge transfer efficiency severely limit the CO2 photoreduction performance of semiconductor heterojunctions. In this work, g-C3N4/Ag@Ag3PO4 S-scheme heterojunction is prepared by an in-situ growth method. The main product for CO2 photoreduction is CO with the selectivity of 97 %. The evolution rate of CO for optimal g-C3N4/Ag@Ag3PO4 heterojunction is 123.8 mu mol g- 1 h-1, which are 8.3and 3.4-fold higher than those of pristine Ag3PO4 and g-C3N4, respectively. It is found that Ag3PO4, Ag, and gC3N4 form strong interacting interfacial structure, in which Ag3PO4 links with Ag nanoparticles through tandem Ohmic contact. More importantly, sigma bonds are formed via hybridization of px orbital for C and N with dx2-y2 orbitals of Ag in g-C3N4/Ag@Ag3PO4 S-scheme heterojunction, establishing an atomic-level dx2-y2(Ag)-px(C,N) charge flow highway. This work provides new viewpoints into the design of heterojunction photocatalysts with high-quality interfaces and highlights the insights of charge transfer behavior in regulating the catalytic activity.
Keyword ：
Charge transfer channel Charge transfer channel CO 2 photoreduction CO 2 photoreduction Interface Interface S-scheme S-scheme
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| GB/T 7714 | Qin, Jianyu , Zhao, Mengyue , Zhang, Yanfeng et al. In situ synthesis of g-C3N4/Ag@Ag3PO4 S-scheme heterostructure with tandem ohmic- and d-p bond-junction for photocatalytic reduction of CO2 [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 353 . |
| MLA | Qin, Jianyu et al. "In situ synthesis of g-C3N4/Ag@Ag3PO4 S-scheme heterostructure with tandem ohmic- and d-p bond-junction for photocatalytic reduction of CO2" . | SEPARATION AND PURIFICATION TECHNOLOGY 353 (2024) . |
| APA | Qin, Jianyu , Zhao, Mengyue , Zhang, Yanfeng , Shen, Jinni , Wang, Xuxu . In situ synthesis of g-C3N4/Ag@Ag3PO4 S-scheme heterostructure with tandem ohmic- and d-p bond-junction for photocatalytic reduction of CO2 . | SEPARATION AND PURIFICATION TECHNOLOGY , 2024 , 353 . |
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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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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 C-1 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 mu mol 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.
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| GB/T 7714 | Lin, Min , Cai, Qing , Xiao, Zhen 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, Min 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, Min , Cai, Qing , Xiao, Zhen , Chen, Hui , Wang, Bing , Qiu, Chengwei 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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