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学者姓名:沈锦妮

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Close π-π stacking facilitated intermolecular charge separation in self-assembled perylene monoimide for photocatalytic hydrogen production SCIE
期刊论文 | 2025 , 44 (6) | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
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Abstract :

The tightness of pi-pi stacking in supramolecular organic semiconductors plays a crucial role in governing the spatial separation and migration dynamics of photogenerated charge carriers, ultimately determining their photocatalytic performance. To achieve close pi-pi stacking, the suitable design of molecular structure is essential. Therefore, two isomers of pyridine carboxylic acid-modified perylene monoimide (PMI) were designed and synthesized, namely PM5A and PM6A. In aqueous solution, these molecules self-assemble into aggregates, which exhibit distinct stacking properties and optical characteristics. Upon photoexcitation, the loose pi-pi stacking of PM5A favors the generation of charge-transfer excitons (CTEs) over charge-separation excitons (CSEs). In contrast, PM6A, stabilized by intermolecular hydrogen bonds and possessing close pi-pi stacking, undergoes efficient charge separation (CS) to produce CSEs within 4.5 picoseconds. When incorporated into metal-insulator-semiconductor (MIS) photosystems with polyvinylpyrrolidone (PVP)-capped Pt, the Pt/PVP/PM6A system demonstrates a hydrogen evolution rate (HER) of 8100 mu mol g(-1) h(-1), nearly five times higher than that of the Pt/PVP/PM5A system. Additionally, the maximum apparent quantum efficiency (AQE) reaches approximately 2.1% under irradiation with light of a single wavelength of lambda = 425 nm.

Keyword :

Hydrogen evolution Hydrogen evolution Perylene monoimide Perylene monoimide Photocatalysis Photocatalysis pi-pi stacking pi-pi stacking Supramolecular semiconductor Supramolecular semiconductor

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GB/T 7714 Wu, Shuhong , Han, Wanying , Wang, Ying et al. Close π-π stacking facilitated intermolecular charge separation in self-assembled perylene monoimide for photocatalytic hydrogen production [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2025 , 44 (6) .
MLA Wu, Shuhong et al. "Close π-π stacking facilitated intermolecular charge separation in self-assembled perylene monoimide for photocatalytic hydrogen production" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 44 . 6 (2025) .
APA Wu, Shuhong , Han, Wanying , Wang, Ying , Zhuang, Yan , Niu, Hui , Li, Lurong et al. Close π-π stacking facilitated intermolecular charge separation in self-assembled perylene monoimide for photocatalytic hydrogen production . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2025 , 44 (6) .
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Inter-layer multi-material powder bed fusion additive manufacturing of a chainmail-like 3D interlocking bonding structure SCIE
期刊论文 | 2025 , 20 (1) | VIRTUAL AND PHYSICAL PROTOTYPING
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Abstract :

Multi-material additive manufacturing (AM) has enabled on-demand material integration by combining distinct properties and functionalities to achieve performance unattainable with single materials, while significantly enhancing design freedom. However, high-precision multi-material AM still presents substantial challenges. Herein, a 3D interlocked chainmail-like Ti64/CP-Ti bioinspired composite with metallurgical bonding interfaces was fabricated via inter-layer multi-material laser powder bed fusion (LPBF) AM. The composite exhibits numerous 100-mu m-scale structural features, reflecting cross-scale complexity, enhanced precision, and advanced manufacturing capabilities. Tensile tests showed that under 0 degrees loading conditions, the composite achieved strength of 875 +/- 21 MPa (80.5% higher than CP-Ti) and ductility of 7.4 +/- 1.6% elongation (28.5% higher than Ti64). Finite element analysis incorporating a modified Johnson-Cook (JC) model reveals that off-axis loading (22.5 degrees/45 degrees) leads to performance degradation due to (1) diminished load-transfer efficiency of the Ti64 skeleton and (2) severe interfacial shear localisation, where shear stresses exceed 240 MPa at 20s(45 degrees loading) and propagate extensively with strain. Cross-interface microhardness mapping indicates powder-spreading-direction-dependent hardness variations. This work establishes a paradigm for bioinspired anisotropic engineering composites (numerous 100-mu m-scale structural features), where Ti64 governs strength via architectural control while CP-Ti enhances damage tolerance through strain delocalisation, offering direct implications for load-adaptive aerospace structures.

Keyword :

chainmail chainmail interfacial bonding interfacial bonding laser powder bed fusion laser powder bed fusion Multi-material additive manufacturing Multi-material additive manufacturing titanium composites titanium composites

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GB/T 7714 Lin, Zixiong , Wu, Hongchun , Zhang, Zheng et al. Inter-layer multi-material powder bed fusion additive manufacturing of a chainmail-like 3D interlocking bonding structure [J]. | VIRTUAL AND PHYSICAL PROTOTYPING , 2025 , 20 (1) .
MLA Lin, Zixiong et al. "Inter-layer multi-material powder bed fusion additive manufacturing of a chainmail-like 3D interlocking bonding structure" . | VIRTUAL AND PHYSICAL PROTOTYPING 20 . 1 (2025) .
APA Lin, Zixiong , Wu, Hongchun , Zhang, Zheng , Huang, Jianghong , Lin, Wenxiong , Shao, Hailong et al. Inter-layer multi-material powder bed fusion additive manufacturing of a chainmail-like 3D interlocking bonding structure . | VIRTUAL AND PHYSICAL PROTOTYPING , 2025 , 20 (1) .
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Inter-layer multi-material powder bed fusion additive manufacturing of a chainmail-like 3D interlocking bonding structure Scopus
期刊论文 | 2025 , 20 (1) | Virtual and Physical Prototyping
Inter-layer multi-material powder bed fusion additive manufacturing of a chainmail-like 3D interlocking bonding structure EI
期刊论文 | 2025 , 20 (1) | Virtual and Physical Prototyping
Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder SCIE
期刊论文 | 2025 , 64 (9) | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
WoS CC Cited Count: 4
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Abstract :

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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Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder Scopus
期刊论文 | 2025 , 64 (9) | Angewandte Chemie - International Edition
Decoupling H2 and O2 Release in Particulate Photocatalytic Overall Water Splitting Using a Reversible O2 Binder EI
期刊论文 | 2025 , 64 (9) | Angewandte Chemie - International Edition
Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution SCIE
期刊论文 | 2025 , 443 | JOURNAL OF CATALYSIS
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Abstract :

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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Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution Scopus
期刊论文 | 2025 , 443 | Journal of Catalysis
Non-stoichiometric problem of photocatalytic water splitting on γ-Ga2O3: Cause and solution EI
期刊论文 | 2025 , 443 | Journal of Catalysis
Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy SCIE
期刊论文 | 2025 , 447 | JOURNAL OF CATALYSIS
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Abstract :

The photocatalytic nonoxidative coupling of methane (CH4) is crucial for sustainable energy production and chemical synthesis, however, a key challenge in advancing this process lies in the development of efficient and highly selective catalytic systems. In this study, we employ an in situ thermally induced strategy to promote the in-situ growth of oxygen vacancies (VO) for constructing a high-density In-VO-In-OH frustrated Lewis pairs (FLP) on Ag/In(OH)3-InOOH (Ag/InOxHy). Our results demonstrate that FLP can effectively polarize C-H bonds, while Ag nanoparticles serve as electron acceptors, significantly reducing the recombination of photogenerated carriers and enhancing the catalytic performance of methane coupling. Benefiting from the high density of FLP and photothermal synergistic effect, we achieve a remarkable C2H6 yield of 339.2 mu mol gcat flow methane atmosphere. Notably, in-situ electron paramagnetic resonance analysis not only validates this innovative strategy but also reveals a new mechanism of oxygen vacancy recycling which showcases its great potential to advance other photocatalytic processes.

Keyword :

High-density frustrated Lewis pairs High-density frustrated Lewis pairs In(OH)3 /InOOH In(OH)3 /InOOH In-situ growth of oxygen vacancies In-situ growth of oxygen vacancies Non-oxidative coupling of methane Non-oxidative coupling of methane Photothermal effect Photothermal effect

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GB/T 7714 Yan, Ziyuan , Li, Xiaoning , Guan, Xinwei et al. Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy [J]. | JOURNAL OF CATALYSIS , 2025 , 447 .
MLA Yan, Ziyuan et al. "Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy" . | JOURNAL OF CATALYSIS 447 (2025) .
APA Yan, Ziyuan , Li, Xiaoning , Guan, Xinwei , Wang, Zhaoliang , Shen, Jinni , Yan, Tingjiang et al. Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy . | JOURNAL OF CATALYSIS , 2025 , 447 .
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Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy EI
期刊论文 | 2025 , 447 | Journal of Catalysis
Boosting photothermal catalytic non-oxidative methane coupling by high-density frustrated Lewis pairs in Ag/InOxHy Scopus
期刊论文 | 2025 , 447 | Journal of Catalysis
One-pot synthesis of transition-metal-sulfides decorated CdS by low-temperature KSCN flux: An effective route to strengthen the interface for enhanced photocatalytic H2 evolution SCIE
期刊论文 | 2025 , 689 | JOURNAL OF COLLOID AND INTERFACE SCIENCE
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Abstract :

The performance of decorated photocatalysts is highly dependent on the interfacial contact between the cocatalyst and the substrate photocatalyst, which is essentially determined by their fabrication routes. Herein, a simple one-pot preparation method based on low-temperature KSCN flux was developed for the synthesis of sulfide photocatalysts with MS/CdS (MS = CoS2, NiS2, Cu1.8S, SnS2, MoS2, and WS2) as prototypes. The results indicate that a sulfidation of Cd2+ and the cocatalyst precursors can be achieved successively in the reaction system, which facilitates the formation of a welded interface as the cocatalysts can grow epitaxially on the formed CdS surface. The KSCN flux serves not only as a reaction medium but also as S2- precursor. Most of the MS (except for WS2) could be successfully fabricated and deposited in situ on CdS. However, only the transition- metal-sulfides (TMSs, MoS2, CoS2, and NiS2) decorated samples showed enhanced photocatalytic H2 evolution reaction (HER) performance and the activities decreased in the order of MoS2 > CoS2 > NiS2. The sample loaded with 1 %MoS2 demonstrated the highest activity, which was 25 times higher than that of the pristine CdS. The superior HER performance could be ascribed to the loading of the active MoS2 sites for HER and the intimate tandem type I (between CdS and 2H-MoS2) and Schottky (between 2H- and 1T-MoS2) junctions for separation of photoinduced charge carriers. Compared to the conventional preparation methods, the developed one-pot flux route demonstrates remarkable advantages in fabricating highly efficient MoS2/CdS photocatalyst besides its convenience, versatility, and scalability. We believe that, in addition to CdS, the developed route can also be applied to synthesize other sulfide-based photocatalysts.

Keyword :

Hydrogen evolution Hydrogen evolution KSCN flux KSCN flux One-pot synthesis One-pot synthesis Photocatalysis Photocatalysis

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GB/T 7714 Fan, Yuge , You, Aichun , Fu, Xianliang et al. One-pot synthesis of transition-metal-sulfides decorated CdS by low-temperature KSCN flux: An effective route to strengthen the interface for enhanced photocatalytic H2 evolution [J]. | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 689 .
MLA Fan, Yuge et al. "One-pot synthesis of transition-metal-sulfides decorated CdS by low-temperature KSCN flux: An effective route to strengthen the interface for enhanced photocatalytic H2 evolution" . | JOURNAL OF COLLOID AND INTERFACE SCIENCE 689 (2025) .
APA Fan, Yuge , You, Aichun , Fu, Xianliang , Shen, Jinni , Zhao, Xuan , Yang, Lei et al. One-pot synthesis of transition-metal-sulfides decorated CdS by low-temperature KSCN flux: An effective route to strengthen the interface for enhanced photocatalytic H2 evolution . | JOURNAL OF COLLOID AND INTERFACE SCIENCE , 2025 , 689 .
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One-pot synthesis of transition-metal-sulfides decorated CdS by low-temperature KSCN flux: An effective route to strengthen the interface for enhanced photocatalytic H2 evolution Scopus
期刊论文 | 2025 , 689 | Journal of Colloid and Interface Science
One-pot synthesis of transition-metal-sulfides decorated CdS by low-temperature KSCN flux: An effective route to strengthen the interface for enhanced photocatalytic H2 evolution EI
期刊论文 | 2025 , 689 | Journal of Colloid and Interface Science
Spherical micro-heterostructured Bi2MoO6/Mo-Bi2O3 with interfacial oxygen vacancies enabling efficient photocatalytic NH3 production from N2 and H2O SCIE
期刊论文 | 2025 , 15 (18) , 5480-5490 | CATALYSIS SCIENCE & TECHNOLOGY
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Abstract :

Photocatalytic nitrogen fixation under mild conditions remains an open challenge due to the low carrier separation efficiency and discrete active sites of conventional photocatalysts. Defect engineering and heterojunctions have emerged as effective strategies to address these issues by enhancing charge carrier mobility and increasing the number of active sites for nitrogen activation. In this study, spherical Bi2MoO6/Mo-Bi2O3 composite photocatalysts with different Mo/Bi ratios are reported to be photocatalytically active for ammonia synthesis from N2 and H2O under full-spectrum light. Bi2MoO6/Mo-Bi2O3 with a Mo/Bi ratio of 24/100 shows the highest activity, with an ammonia production rate as high as 141.93 mu mol g-1 h-1. This high photocatalytic activity is attributed to the formation of a micro-heterojunction of Bi2MoO6 on Mo-doped Bi2O3 and the presence of oxygen vacancies (Ov) at the interfacial surface between two phases. The Ov enhances the adsorption and activation of N2 and H2O molecules, while the micro-heterojunction improves separation efficiency of photogenerated charges. More importantly, N2 molecules and H2O molecules could be adsorbed at Bi3+ and Mo5+ sites at two sides of the Ov at the interfacial surface between Bi2MoO6 and Mo-Bi2O3 to form a N2/Bi-OV-Mo/H2O cyclic transition state. Upon illumination, the photogenerated electrons and holes transfer to the Bi and Mo sites, where they are captured by N2 and H2O molecules, respectively. In this way, N2 and H2O are transformed step by step into NH3 and O2. This work underscores the synergistic roles of the micro-heterojunction and oxygen vacancies of Bi2MoO6/Bi2O3 for enhancing photocatalytic nitrogen fixation. The proposed mechanism offers valuable insights for designing high-performance photocatalysts for photocatalytic ammonia production.

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GB/T 7714 Wu, Dan , Hong, Lu , Gu, Xin et al. Spherical micro-heterostructured Bi2MoO6/Mo-Bi2O3 with interfacial oxygen vacancies enabling efficient photocatalytic NH3 production from N2 and H2O [J]. | CATALYSIS SCIENCE & TECHNOLOGY , 2025 , 15 (18) : 5480-5490 .
MLA Wu, Dan et al. "Spherical micro-heterostructured Bi2MoO6/Mo-Bi2O3 with interfacial oxygen vacancies enabling efficient photocatalytic NH3 production from N2 and H2O" . | CATALYSIS SCIENCE & TECHNOLOGY 15 . 18 (2025) : 5480-5490 .
APA Wu, Dan , Hong, Lu , Gu, Xin , Liu, Yanan , Li, Haohong , Shen, Jinni et al. Spherical micro-heterostructured Bi2MoO6/Mo-Bi2O3 with interfacial oxygen vacancies enabling efficient photocatalytic NH3 production from N2 and H2O . | CATALYSIS SCIENCE & TECHNOLOGY , 2025 , 15 (18) , 5480-5490 .
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Spherical micro-heterostructured Bi2MoO6/Mo-Bi2O3 with interfacial oxygen vacancies enabling efficient photocatalytic NH3 production from N2 and H2O EI
期刊论文 | 2025 , 15 (18) , 5480-5490 | Catalysis Science and Technology
Probing local structure and electronic structure of α-Fe2O3/g-C3N4 S-scheme heterojunctions for boosting CO2 photoreduction SCIE
期刊论文 | 2025 , 685 , 1109-1121 | JOURNAL OF COLLOID AND INTERFACE SCIENCE
WoS CC Cited Count: 6
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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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Probing local structure and electronic structure of α-Fe2O3/g-C3N4 S-scheme heterojunctions for boosting CO2 photoreduction Scopus
期刊论文 | 2025 , 685 , 1109-1121 | Journal of Colloid and Interface Science
Probing local structure and electronic structure of α-Fe2O3/g-C3N4 S-scheme heterojunctions for boosting CO2 photoreduction EI
期刊论文 | 2025 , 685 , 1109-1121 | Journal of Colloid and Interface Science
Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH SCIE
期刊论文 | 2025 , 35 (25) | ADVANCED FUNCTIONAL MATERIALS
WoS CC Cited Count: 2
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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 , 35 (25) .
MLA Xiao, Zhen et al. "Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH" . | ADVANCED FUNCTIONAL MATERIALS 35 . 25 (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 , 35 (25) .
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Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH EI
期刊论文 | 2025 , 35 (25) | Advanced Functional Materials
Synergetic Atom-Island and Metal Alloy Triggering Tandem Reaction for CH4 Photooxidation to CH3OH Scopus
期刊论文 | 2025 , 35 (25) | Advanced Functional Materials
Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction SCIE
期刊论文 | 2025 , 398 | FUEL
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Abstract :

Controlling the crystallinity and microstructure of a semiconductor photocatalyst serves as an effective means to boost its photocatalytic performance through improving the charge transfer and separation, enhancing the light absorption, or maneuvering the surface reactions. Nevertheless, the internal pores in aerogel materials inevitably collapse during the traditional high temperature crystallization process, significantly reducing the porous structure and specific surface area (SSA). Herein, microsphere ZnO aerogels have been successfully fabricated for photoreduction of CO2 using a cooperative strategy of sol-gel method, solvothermal crystallization and cryodesiccation. The obtained aerogel has a large SSA and high crystallinity. Compared with the commercial ZnO powder, the ZnO aerogel microsphere exhibits about 4-fold increase in specific surface area, leading to an increased contact surface between the photocatalyst and the reactant. At the same time, ZnO aerogel with microsphere morphology possesses high light-harvesting and intrapore light reflecting capabilities, demonstrating enhanced optical utilization. Modulation of the crystallinity of ZnO aerogel facilitated the incorporation of defect engineering (zinc defects (Zni) and oxygen vacancies (Vo)). As a result, ZnO aerogel microsphere exhibits a 5-fold higher products production rate than ZnO powder for photocatalytic CO2 reactions due to the synergistic effect of appropriate crystallinity and microsphere appearance. It is hoped that this work may provide some insights to tune the catalyst performance through crystallinity and morphology.

Keyword :

CO2 reduction reaction CO2 reduction reaction Crystallization Crystallization Photocatalysis Photocatalysis Solvothermal Solvothermal ZnO aerogel microspheres ZnO aerogel microspheres

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GB/T 7714 Xu, Xiaochao , Zou, Jiaxin , Xiao, Zhen et al. Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction [J]. | FUEL , 2025 , 398 .
MLA Xu, Xiaochao et al. "Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction" . | FUEL 398 (2025) .
APA Xu, Xiaochao , Zou, Jiaxin , Xiao, Zhen , Zhang, Jiangjie , Wang, Bing , Jiang, Jianing et al. Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction . | FUEL , 2025 , 398 .
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Crystalline ZnO aerogel microspheres for boosting photocatalytic CO2 reduction Scopus
期刊论文 | 2025 , 398 | Fuel
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