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学者姓名：邢万东
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Abstract ：
Constructing heterointerfaces with space charge areas can effectively drive carrier transport. However, it is difficult to further enhance the interfacial bond strength to improve the built-in potential difference across the interface by directly modulating the interfacial atomic configuration. Herein, we have directly regulated the atomic structures of ZnO/CoO heterointerfaces by means of the phase transition of the rocksalt CoO to spinel Co3O4 under a high-energy electron beam. The results show that irradiation of electron beams can drive the orderly migration and aggregation of Co vacancies as well as the rearrangement of lattice Co atoms from octahedral sites to tetrahedral sites, causing the formation of spinel Co3O4. DFT calculations demonstrate that O atoms adjected to four-coordinated Co atoms are strongly coupled with the Zn atoms, enhancing interfacial polarization to facilitate the charge transfer. This finding provides a novel idea for the design of heterojunctions with high-efficiency charge transport.
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| GB/T 7714 | Zhao, Quanpan , Zhao, Yanan , Wang, Mingyue et al. Atomic Manipulation of Metal Oxide Heterointerfaces by Electron Beam Illumination [J]. | JOURNAL OF PHYSICAL CHEMISTRY LETTERS , 2025 , 16 (8) : 1865-1872 . |
| MLA | Zhao, Quanpan et al. "Atomic Manipulation of Metal Oxide Heterointerfaces by Electron Beam Illumination" . | JOURNAL OF PHYSICAL CHEMISTRY LETTERS 16 . 8 (2025) : 1865-1872 . |
| APA | Zhao, Quanpan , Zhao, Yanan , Wang, Mingyue , Xue, Sikang , Yu, Rong , Xing, Wandong . Atomic Manipulation of Metal Oxide Heterointerfaces by Electron Beam Illumination . | JOURNAL OF PHYSICAL CHEMISTRY LETTERS , 2025 , 16 (8) , 1865-1872 . |
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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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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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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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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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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 , 64 (7) . |
| MLA | Ye, Hanfeng et al. "Sabatier Optimal of Mn-N4 Single Atom Catalysts for Selective Oxidative Desulfurization" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 7 (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 , 64 (7) . |
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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 , 64 (5) . |
| 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 64 . 5 (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 , 64 (5) . |
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Poly (heptazine imide) (PHI), a classic 2D polymeric photocatalyst, represents a promising organic semiconductor for photocatalytic overall water splitting (POWS). However, since the key bottleneck in POWS of PHI remains unclear, its quantum efficiency of POWS is extremely restrained. To identify the key obstacle in POWS on the PHI, a series of PHI with different stacking modes is synthesized by tuning interlayer cations. The structural characterizations revealed that tuning the interlayer cations of PHI can induce rearrangements in interlayer stacking modes. Additionally, charge carriers dynamics uncover that optimizing the interlayer stacking modes of PHI can promote exciton diffusion and prolong the photoexcited electron lifetimes, thus improving the concentration of surface-reaching charge. More importantly, this confirms that the POWS activity of PHI is closely correlated with the interlayer stacking modes. This work offers new insight into structural regulation for governing charge-transport dynamics and the activity of 2D polymeric photocatalysts.
Keyword ：
charge transport charge transport interlayer stacking modes interlayer stacking modes overall water splitting overall water splitting photocatalysis photocatalysis poly (heptazine imide) poly (heptazine imide)
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| GB/T 7714 | Pan, Zhiming , Zhang, Guigang , Zhang, Xirui et al. Unveiling the Key Obstacle in Photocatalytic Overall Water Splitting Reaction on Poly (heptazine imide) Semiconductors [J]. | SMALL , 2024 , 21 (1) . |
| MLA | Pan, Zhiming et al. "Unveiling the Key Obstacle in Photocatalytic Overall Water Splitting Reaction on Poly (heptazine imide) Semiconductors" . | SMALL 21 . 1 (2024) . |
| APA | Pan, Zhiming , Zhang, Guigang , Zhang, Xirui , Xing, Wandong , Zheng, Dandan , Wang, Sibo et al. Unveiling the Key Obstacle in Photocatalytic Overall Water Splitting Reaction on Poly (heptazine imide) Semiconductors . | SMALL , 2024 , 21 (1) . |
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