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学者姓名：邢万东
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Abstract ：
The artificial photosynthesis of H2O2 from water and oxygen using semiconductor photocatalysts is attracting increasing levels of attention owing to its green, environmentally friendly, and energy-saving characteristics. Although covalent organic frameworks (COFs) are promising materials for promoting photocatalytic H2O2 production owing to their structural and functional diversity, they typically suffer from low charge-generation and -transfer efficiencies as well as rapid charge recombination, which restricts their use as catalysts for photocatalytic H2O2 production. Herein, we report a strategy for anchoring vinyl moieties to a COF skeleton to facilitate charge separation and migration, thereby promoting photocatalytic H2O2 generation. This vinyl-group-bearing COF photocatalyst exhibits a H2O2 -production rate of 84.5 mu mol h(-1) (per 10 mg), which is ten-times higher than that of the analog devoid of vinyl functionality and superior to most reported COF photocatalysts. Both experimental and theoretical studies provide deep insight into the origin of the improved photocatalytic performance. These findings are expected to facilitate the rational design and modification of organic semiconductors for use in photocatalytic applications.
Keyword ：
Charge separation Charge separation Covalent organic frameworks Covalent organic frameworks H2O2 production H2O2 production Photocatalysts Photocatalysts Vinyl groups Vinyl groups
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| GB/T 7714 | Yu, Hong , Zhang, Fengtao , Chen, Qian et al. Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (21) . |
| MLA | Yu, Hong et al. "Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 21 (2024) . |
| APA | Yu, Hong , Zhang, Fengtao , Chen, Qian , Zhou, Pan-Ke , Xing, Wandong , Wang, Sibo et al. Vinyl-Group-Anchored Covalent Organic Framework for Promoting the Photocatalytic Generation of Hydrogen Peroxide . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (21) . |
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Hybridizing two heterocomponents to construct a built-in electric field (BIEF) at the interface represents a significant strategy for facilitating charge separation in carbon dioxide (CO2)-photoreduction. However, the unidirectional nature of BIEFs formed by various low-dimensional materials poses challenges in adequately segregating the photogenerated carriers produced in bulk. In this study, leveraging zinc oxide (ZnO) nanodisks, a sulfurization reaction is employed to fabricate Z-scheme ZnO/zinc sulfide (ZnS) heterojunctions featuring a multiple-order BIEF. These heterojunctions reveal distinctive interfacial structures characterized by two semicoherent phase boundaries. The cathodoluminescence 2D maps and density functional theory calculation results demonstrate that the direction of the multiple-order BIEF spans from ZnS to ZnO. This directional alignment significantly fosters the spatial separation of photogenerated electrons and holes within ZnS nanoparticles and enhances CO2-to-carbon monoxide photoreduction performance (3811.7 mu mol h(-1) g(-1)). The findings present a novel pathway for structurally designing BIEFs within heterojunctions, while providing fresh insights into the migratory behavior of photogenerated carriers across interfaces.
Keyword ：
built-in electric field built-in electric field CO2 photoreduction CO2 photoreduction heterojunctions heterojunctions interfacial structures interfacial structures photocatalysis photocatalysis
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| GB/T 7714 | Xue, Sikang , Tang, Hao , Shen, Min et al. Establishing Multiple-Order Built-In Electric Fields Within Heterojunctions to Achieve Photocarrier Spatial Separation [J]. | ADVANCED MATERIALS , 2024 , 36 (16) . |
| MLA | Xue, Sikang et al. "Establishing Multiple-Order Built-In Electric Fields Within Heterojunctions to Achieve Photocarrier Spatial Separation" . | ADVANCED MATERIALS 36 . 16 (2024) . |
| APA | Xue, Sikang , Tang, Hao , Shen, Min , Liang, Xiaocong , Li, Xiaoyan , Xing, Wandong et al. Establishing Multiple-Order Built-In Electric Fields Within Heterojunctions to Achieve Photocarrier Spatial Separation . | ADVANCED MATERIALS , 2024 , 36 (16) . |
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Surface atomic structure is closely related to the physical and chemical properties of materials. Although cupric oxide (CuO) surfaces have been widely reported, to the best of our knowledge, the low Miller index and easily exposed CuO(0 0 1) surface has not been yet investigated in experiments at the atomic scale. Herein, for the first time, we report the atomic structures of CuO(0 0 1) surface combining aberration-corrected scanning transmission electron microscopy and first-principles calculations. Interestingly, akin to the (1 1 1) surfaces of FeO, CoO and NiO, a unusual tetrahedral reconstructed structure was revealed for the CuO(0 0 1) surface. The low energy barrier from square-planar to tetrahedral coordination for the surface CuO4 unit was found by the climbing-image nudged-elastic band method. © 2024 Elsevier B.V.
Keyword ：
Atoms Atoms Cobalt compounds Cobalt compounds Copper oxides Copper oxides Crystal atomic structure Crystal atomic structure High resolution transmission electron microscopy High resolution transmission electron microscopy Iron oxides Iron oxides Nickel oxide Nickel oxide Scanning electron microscopy Scanning electron microscopy
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| GB/T 7714 | Wang, Mingyue , Li, Xiaoyan , Zeng, Xiangkai et al. Surface reconstruction in the CuO(001) surface: From square-planar to tetrahedral coordination for CuO4 unit [J]. | Applied Surface Science , 2024 , 670 . |
| MLA | Wang, Mingyue et al. "Surface reconstruction in the CuO(001) surface: From square-planar to tetrahedral coordination for CuO4 unit" . | Applied Surface Science 670 (2024) . |
| APA | Wang, Mingyue , Li, Xiaoyan , Zeng, Xiangkai , Zhao, Quanpan , Zhang, Mengmeng , Meng, Fanyan et al. Surface reconstruction in the CuO(001) surface: From square-planar to tetrahedral coordination for CuO4 unit . | Applied Surface Science , 2024 , 670 . |
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Fluorite-perovskite heterointerfaces garner great interest for enhanced ionic conductivity for application in electronic and energy devices. However, the origin of observed enhanced ionic conductivity as well as the details of the atomic structure at these interfaces remain elusive. Here, systematic, multi-stoichiometry computational searches and experimental investigations are performed to obtain stable and exact atomic structures of interfaces between CeO2 and SrTiO3-two archetypes of the corresponding structural families. Local reconstructions take place at the interface because of mismatched lattices. TiO2 terminated SrTiO3 causes a buckled rock salt CeO interface layer to emerge. In contrast, SrO terminated SrTiO3 maintains the fluorite structure at the interface compensated by a partially occupied anion lattice. Moderate enhancement in oxygen diffusion is found along the interface by simulations, yet evidence to support further significant enhancement is lacking. Our findings demonstrate the control of interface termination as an effective pathway to achieve desired device performance.
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| GB/T 7714 | Zhu, Bonan , Schusteritsch, Georg , Li, Weiwei et al. Structure and ionic conduction enhancement mechanisms at CeO2/SrTiO3 heterointerfaces [J]. | APPLIED PHYSICS REVIEWS , 2024 , 11 (2) . |
| MLA | Zhu, Bonan et al. "Structure and ionic conduction enhancement mechanisms at CeO2/SrTiO3 heterointerfaces" . | APPLIED PHYSICS REVIEWS 11 . 2 (2024) . |
| APA | Zhu, Bonan , Schusteritsch, Georg , Li, Weiwei , Xing, Wandong , Yu, Rong , Pickard, Chris J. et al. Structure and ionic conduction enhancement mechanisms at CeO2/SrTiO3 heterointerfaces . | APPLIED PHYSICS REVIEWS , 2024 , 11 (2) . |
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Despite the pivotal role of molecular oxygen (O-2) activation in artificial photosynthesis, the activation efficiency is often restricted by sluggish exciton dissociation and charge transfer kinetics within polymer photocatalysts. Herein, we propose two tetrathiafulvalene (TTF)-based imine-linked covalent organic frameworks (COFs) with tailored donor-acceptor (D-A) structures, TTF-PDI-COF and TTF-TFPP-COF, to promote O-2 activation. Because of enhanced electron push-pull interactions that facilitated charge separation and transfer behavior, TTF-PDI-COF exhibited superior photocatalytic activity in electron-induced O-2 activation reactions over TTF-TFPP-COF under visible light irradiation, including the photosynthesis of (E)-3-amino-2-thiocyano-alpha,beta-unsaturated compounds and H2O2. These findings highlight the significant potential of the rational design of COFs with D-A configurations as suitable candidates for advanced photocatalytic applications.
Keyword ：
Covalent organic frameworks Covalent organic frameworks Donor-acceptor polymers Donor-acceptor polymers H2O2 production H2O2 production Molecular oxygen activation Molecular oxygen activation Photocatalysis Photocatalysis
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| GB/T 7714 | Xu, Hetao , Xia, Shuling , Li, Chunlei et al. Programming Tetrathiafulvalene-Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
| MLA | Xu, Hetao et al. "Programming Tetrathiafulvalene-Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 29 (2024) . |
| APA | Xu, Hetao , Xia, Shuling , Li, Chunlei , Li, Yang , Xing, Wandong , Jiang, Yi et al. Programming Tetrathiafulvalene-Based Covalent Organic Frameworks for Promoted Photoinduced Molecular Oxygen Activation . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (29) . |
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Defect engineering has been widely applied in semiconductors to improve photocatalytic properties by altering the surface structures. This study is about the transformation of inactive WO 3 nanosheets to a highly effective CO 2 - to - CH 4 conversion photocatalyst by introducing surface - ordered defects in abundance. The nonstoichiometric WO 3 - x samples were examined by using aberration - corrected electron microscopy. Results unveil abundant surface - ordered terminations derived from the periodic {013} stacking faults with a defect density of 20.2%. The {002} surface - ordered line defects are the active sites for fixation CO 2 , transforming the inactive WO 3 nanosheets into a highly active catalyst (CH 4 : O 2 = 8.2: 16.7 mu mol h -1 ). We believe that the formation of the W - O - C - W - O species is a critical step in the catalytic pathways. This work provides an atomic - level comprehension of the structural defects of catalysts for activating small molecules.
Keyword ：
CO 2 conversion CO 2 conversion induced polarization induced polarization photocatalysis photocatalysis surface- ordered defects surface- ordered defects unsaturated coordination unsaturated coordination
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| GB/T 7714 | Xue, Sikang , Wei, Changgeng , Shen, Min et al. Enriching surface- ordered defects on WO3 for photocatalytic CO2-to-CH4 conversion by water [J]. | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA , 2024 , 121 (18) . |
| MLA | Xue, Sikang et al. "Enriching surface- ordered defects on WO3 for photocatalytic CO2-to-CH4 conversion by water" . | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA 121 . 18 (2024) . |
| APA | Xue, Sikang , Wei, Changgeng , Shen, Min , Liang, Xiaocong , Wang, Jiali , Yang, Can et al. Enriching surface- ordered defects on WO3 for photocatalytic CO2-to-CH4 conversion by water . | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA , 2024 , 121 (18) . |
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Strong excitonic effects are common in organic conjugated polymer semiconductors, severely hindering the generation of free charge carriers for conducting photocatalysis. Therefore, exploring new channels to modulate exciton dissociation in polymers is far-reaching in facilitating photocatalysis. A series of B-N Lewis pair functionalized conjugated polymers have been developed to minimize exciton effects by modulating charge transfer pathways. Theoretical studies have shown that introducing B-N Lewis pairs can dramatically increase the distance of charge transfer (D index) and the amount of electron transfer and reduce the Coulomb attraction energy (EC), which contributes to breaking the equilibrium of the coexistence of excitons and charge carriers. Further experimental results show that the singlet excitons are efficiently dissociated into more free-charge carriers under photoexcitation to participate in surface reactions. The optimized polymer PyPBM shows an exponential increase in photocatalytic hydrogen and hydrogen peroxide production performance by visible light illumination.
Keyword ：
B-N Lewis pair B-N Lewis pair Conjugated polymers Conjugated polymers Exciton binding energy Exciton binding energy Exciton effects Exciton effects Photocatalyst Photocatalyst
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| GB/T 7714 | Ru, Chenglong , Nie, Xiaoyu , Lan, Zhi-An et al. Regulation of Exciton Effects in Functionalized Conjugated Polymers by B-N Lewis Pairs for Visible-Light Photocatalysis [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
| MLA | Ru, Chenglong et al. "Regulation of Exciton Effects in Functionalized Conjugated Polymers by B-N Lewis Pairs for Visible-Light Photocatalysis" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024) . |
| APA | Ru, Chenglong , Nie, Xiaoyu , Lan, Zhi-An , Pan, Zhiming , Xing, Wandong , Wang, Sibo et al. Regulation of Exciton Effects in Functionalized Conjugated Polymers by B-N Lewis Pairs for Visible-Light Photocatalysis . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
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Understanding the relationship of competitive adsorption between reactants is the prerequisite for high activity and selectivity in heterogeneous catalysis, especially the difference between the adsorption energies (E-ads) of two reactive intermediates in Langmuir-Hinshelwood (L-H) models. Using oxidative dehydrogenation of hydrogen sulfide (H2S-ODH) as a probe, we develop various metal single atoms on nitrogen-doped carbon (M-NDC) catalysts for controlling E-ads-H2S, E-ads-O-2 and investigating the difference in activity and selectivity. Combining theoretical and experimental results, a Sabatier relationship between the catalytic performance and E-ads-O-2/E-ads-H2S emerges. Mn-NDC as the optimal catalyst shows excellent H2S conversion (>90 %) and sulfur selectivity (>90 %) in a wide range of O-2 concentrations over 100 h. Such a high-efficiency performance is attributed to appropriate E-ads-H2S and E-ads-O-2 on Mn-N-4 sites, boosting redox cycle between Mn2+ and Mn3+, as well as preferential formation of sulfur. This work provides a fundamental guidance for designing Sabatier optimal catalysts in L-H models.
Keyword ：
high-efficiency reactivity descriptors high-efficiency reactivity descriptors nitrogen-doped carbon nitrogen-doped carbon Sabatier principle Sabatier principle selective oxidative desulfurization selective oxidative desulfurization single atoms single atoms
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| GB/T 7714 | Ye, Hanfeng , Xing, Wandong , Zhao, Fei et al. Sabatier Optimal of Mn-N4 Single Atom Catalysts for Selective Oxidative Desulfurization [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
| MLA | Ye, Hanfeng et al. "Sabatier Optimal of Mn-N4 Single Atom Catalysts for Selective Oxidative Desulfurization" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2024) . |
| APA | Ye, Hanfeng , Xing, Wandong , Zhao, Fei , Wang, Jiali , Yang, Can , Hou, Yidong et al. Sabatier Optimal of Mn-N4 Single Atom Catalysts for Selective Oxidative Desulfurization . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 . |
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Poly (triazine imide) (PTI/Li+Cl-), one of the crystalline versions of polymeric carbon nitrides, holds great promise for photocatalytic overall water splitting. In principle, the photocatalytic activity of PTI/Li+Cl- is closely related to the morphology, which could be reasonably tailored by the modulation of the polycondensation process. Herein, we demonstrate that the hexagonal prisms of PTI/Li+Cl- could be converted to hexagonal nanosheets by adjusting the binary eutectic salts from LiCl/KCl or NaCl/LiCl to ternary LiCl/KCl/NaCl. Results reveal that the extension of in-plane conjugation is preferred, when the polymerisation was performed in the presence of ternary eutectic salts. The hexagonal nanosheets bears longer lifetimes of charge carriers than that of hexagonal prisms due to lower intensity of structure defects and shorter hopping distance of charge carriers along the stacking direction of triazine nanosheets. The optimized hexagonal nanosheets exhibits a record apparent quantum yield value of 25 % (& lambda;=365 nm) for solar hydrogen production by one-step excitation overall water splitting.
Keyword ：
Cocatalysts Cocatalysts Overall Water Splitting Overall Water Splitting Polymer Crystals Polymer Crystals Poly Triazine Imide Poly Triazine Imide Salt Melt Synthesis Salt Melt Synthesis
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| GB/T 7714 | Wang, Qian , Zhang, Guigang , Xing, Wandong et al. Bottom-up Synthesis of Single-Crystalline Poly (Triazine Imide) Nanosheets for Photocatalytic Overall Water Splitting [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (37) . |
| MLA | Wang, Qian et al. "Bottom-up Synthesis of Single-Crystalline Poly (Triazine Imide) Nanosheets for Photocatalytic Overall Water Splitting" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 62 . 37 (2023) . |
| APA | Wang, Qian , Zhang, Guigang , Xing, Wandong , Pan, Zhiming , Zheng, Dandan , Wang, Sibo et al. Bottom-up Synthesis of Single-Crystalline Poly (Triazine Imide) Nanosheets for Photocatalytic Overall Water Splitting . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2023 , 62 (37) . |
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Ruddlesden-Popper (RP) faults in perovskites as one type of the anti-phase boundaries provide a versatile platform to manipulate the magnetic, conducting, and magnetoresistance properties in the complex oxides. Local fine structure at the boundaries containing light atoms is a key factor to understand the underlying structurefunction relationship due to their interfaces mediated effects. In this work, the atomic structure, chemical distribution and electronic structure of typical RP faults in perovskite LaNiO3 and its epitaxial nanocomposite films on a SrTiO3 substrate were systematically investigated combining high-resolution scanning transmission electron microscopy (STEM) and density functional theory (DFT) calculations. Integrated differential phase contrast (iDPC) STEM imaging results demonstrate a NiO2-x-(LaO-LaO)-NiO2-x atomic configuration with content fluctuations of oxygen at the RP faults. Atomic electronic energy loss spectroscopy results and DFT calculations illustrate that Ni cations have mixed valence of Ni2+, Ni3+ at the RP faults accompanying with oxygen environment fluctuations affected by the non-stoichiometric bonding. This study offers a comprehensive route to explore intriguing chemical structures and physical properties in the homointerface structure at the atomic level.
Keyword ：
Atomic structure imaging Atomic structure imaging DFT calculations DFT calculations LaNiO 3 films LaNiO 3 films Ruddlesden-Popper faults Ruddlesden-Popper faults
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| GB/T 7714 | Zhu, Yuanmin , Liao, Ping , Xing, Wandong et al. Revealing direct atomic structure and electrostatic maps of the Ruddlesden-Popper faults in LaNiO3 perovskite [J]. | JOURNAL OF ALLOYS AND COMPOUNDS , 2023 , 969 . |
| MLA | Zhu, Yuanmin et al. "Revealing direct atomic structure and electrostatic maps of the Ruddlesden-Popper faults in LaNiO3 perovskite" . | JOURNAL OF ALLOYS AND COMPOUNDS 969 (2023) . |
| APA | Zhu, Yuanmin , Liao, Ping , Xing, Wandong , Liu, Jiayu , Cui, Jizhe , Jin, Cai et al. Revealing direct atomic structure and electrostatic maps of the Ruddlesden-Popper faults in LaNiO3 perovskite . | JOURNAL OF ALLOYS AND COMPOUNDS , 2023 , 969 . |
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