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学者姓名：喻志阳
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Abstract ：
Oxygen vacancies (OVs) spatially confined on the surface of metal oxide semiconductors are advantageous for photocatalysis, in particular, for O2-involved redox reactions. However, the thermal annealing process used to generate surface OVs often results in undesired bulk OVs within the metal oxides. Herein, a high pressure-assisted thermal annealing strategy has been developed for selectively confining desirable amounts of OVs on the surface of metal oxides, such as tungsten oxide (WO3). Applying a pressure of 1.2 gigapascal (GPa) on WO3 induces significant lattice compression, which would strengthen the W-O bonds and increase the diffusion activation energy for the migration of the O migration. This pressure-induced compression effectively inhibits the formation of bulk OVs, resulting in a high density of surface-confined OVs on WO3. These well-defined surface OVs significantly enhance the photocatalytic activation of O2, facilitating H2O2 production and aerobic oxidative coupling of amines. This strategy holds promise for the defect engineering of other metal oxides, enabling abundant surface OVs for a range of emerged applications.
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| GB/T 7714 | Wang, Xiaoyi , Xue, Sikang , Huang, Meirong et al. Pressure-Induced Engineering of Surface Oxygen Vacancies on Metal Oxides for Heterogeneous Photocatalysis [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (6) : 4945-4951 . |
| MLA | Wang, Xiaoyi et al. "Pressure-Induced Engineering of Surface Oxygen Vacancies on Metal Oxides for Heterogeneous Photocatalysis" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 6 (2025) : 4945-4951 . |
| APA | Wang, Xiaoyi , Xue, Sikang , Huang, Meirong , Lin, Wei , Hou, Yidong , Yu, Zhiyang et al. Pressure-Induced Engineering of Surface Oxygen Vacancies on Metal Oxides for Heterogeneous Photocatalysis . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (6) , 4945-4951 . |
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Photocatalytic ozonation emerges as an appealing approach for wastewater purification. However, the kinetic constraints associated with the charge separation and the ozone activation hinder the advancement of photocatalytic ozonation systems. Herein, we prepared CeO2 photocatalysts with predominantly exposed {110}, {100}, or {111} facets, highlighting the synergy role of crystal facet and oxygen vacancies in manipulating electron transfer and ozone activation. The CeO2-{1 1 0} catalyst exhibits the best efficiency for phenol mineralization (69%) in photocatalytic ozonation. Ex-situ, Quasi-situ, and In-situ characterization of the CeO2 catalysts reveal that facet engineering in the CeO2 catalysts optimizes the electronic properties of the catalysts, thereby enhancing the separation of photogenerated charge carriers and transfer of electrons and holes, which provides more electrons for O3 activation and promotes the formation of reactive oxygen species (ROS). Moreover, facet modulating leads to a change in the density of surface oxygen vacancies. The increased oxygen vacancy density on the CeO2-{1 1 0} surface accelerates the activation of O3 and the formation of adsorbed oxygen (*O), synergistically boosting the production rate of ROS. The present study offers valuable insights into the design of efficient photocatalysts for wastewater purification.
Keyword ：
Crystal facet Crystal facet Oxygen vacancies Oxygen vacancies Photocatalytic ozonation Photocatalytic ozonation Synergistic effect Synergistic effect
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| GB/T 7714 | Yang, Zhou , Xu, Ruizhang , Tao, Huilin et al. Crystal facet and oxygen vacancies synergistically mediate photocatalytic ozonation for organic pollutants removal over CeO2 [J]. | JOURNAL OF CATALYSIS , 2024 , 438 . |
| MLA | Yang, Zhou et al. "Crystal facet and oxygen vacancies synergistically mediate photocatalytic ozonation for organic pollutants removal over CeO2" . | JOURNAL OF CATALYSIS 438 (2024) . |
| APA | Yang, Zhou , Xu, Ruizhang , Tao, Huilin , Yang, Yang , Hou, Yidong , Wang, Ke et al. Crystal facet and oxygen vacancies synergistically mediate photocatalytic ozonation for organic pollutants removal over CeO2 . | JOURNAL OF CATALYSIS , 2024 , 438 . |
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Developing highly effective catalysts for ammonia (NH3) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C-60) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The 'electron buffer' behaviour of C-60 balances the electron density at catalytic transition metal sites and enables the synergistic activation of nitrogen on transition metals in addition to the activation and migration of hydrogen on C-60 sites. As demonstrated in long-term, continuous runs, the C-60-promoting transition metal co-catalysts exhibit higher NH3 synthesis rates than catalysts without C-60. With the involvement of C-60, the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH2. C-60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.
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| GB/T 7714 | Zhang, Yangyu , Peng, Xuanbei , Tian, Han-Rui et al. Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis [J]. | NATURE CHEMISTRY , 2024 , 16 (11) . |
| MLA | Zhang, Yangyu et al. "Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis" . | NATURE CHEMISTRY 16 . 11 (2024) . |
| APA | Zhang, Yangyu , Peng, Xuanbei , Tian, Han-Rui , Yang, Bo , Chen, Zuo-Chang , Li, Jiejie et al. Fullerene on non-iron cluster-matrix co-catalysts promotes collaborative H2 and N2 activation for ammonia synthesis . | NATURE CHEMISTRY , 2024 , 16 (11) . |
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Thermocatalytic nonoxidative ethane dehydrogenation(EDH)is a promising strategy for ethene produc-tion but suffers from intense energy consumption and poor catalyst durability;exploring technology that permits efficient EDH by solar energy remains a giant challenge.Herein,we present that an oxygen va-cancy(Ov)-rich LaVO4(LaV04-Ov)catalyst is highly active and stable for photocatalytic EDH,through a dynamic lattice oxygen(Olatt.)and Ov co-mediated mechanism.Irradiated by simulated sunlight at mild conditions,LaVO4-Ov effectively dehydrogenates undiluted ethane to produce C2H4 and CO with a con-version of 2.3％.By loading a small amount of Pt cocatalyst,the evolution and selectivity of C2H4 are en-hanced to 275 μmol h-1 g-1 and 96.8％.Of note,LaVO4-Ov appears nearly no carbon deposition after the reaction.The isotope tracked reactions reveal that the consumed Olatt.recuperates by exposing the used catalyst with O2,thus establishing a dynamic cycle of Olatt,and achieving a facile catalyst regeneration to preserve its intrinsic activity.The refreshed LaVO4-Ov exhibits superior reusability and delivers a turnover number of about 305.The Ov promotes photo absorption,boosts ethane adsorption/activation,and accel-erates charge separation/transfer,thus improving the photocatalytic efficiency.The possible photocatalytic EDH mechanism is proposed,considering the key intermediates predicted by density functional theory(DFT)and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS).
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| GB/T 7714 | Fen Wei , Weichao Xue , Zhiyang Yu et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst [J]. | 中国化学快报（英文版） , 2024 , 35 (3) : 171-176 . |
| MLA | Fen Wei et al. "Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst" . | 中国化学快报（英文版） 35 . 3 (2024) : 171-176 . |
| APA | Fen Wei , Weichao Xue , Zhiyang Yu , Xue Feng Lu , Sibo Wang , Wei Lin et al. Dynamic cooperations between lattice oxygen and oxygen vacancies for photocatalytic ethane dehydrogenation by a self-restoring LaVO4 catalyst . | 中国化学快报（英文版） , 2024 , 35 (3) , 171-176 . |
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Materials that can provide reliable electromagnetic interference (EMI) shielding in highly oxidative atmosphere at elevated temperature are indispensable in the fast-developing aerospace field. However, most of conductor-type EMI shielding materials such as metals can hardly withstand the high-temperature oxidation, while the conventional dielectric-type materials cannot offer sufficient shielding efficiency in gigahertz (GHz) frequencies. Here, a highly deficient medium-entropy (ME) perovskite ceramic as an efficient EMI shielding material in harsh environment, is demonstrated. The synergistic effect of entropy stabilization and aliovalent substitution on A-site generate abnormally high concentration of Ti and O vacancies that are stable under high-temperature oxidation. Due to the clustering of vacancies, the highly deficient perovskite ceramic exhibits giant complex permittivity and polarization loss in GHz, leading to the specific EMI shielding effectiveness above 30 dB/mm in X-band even after 100 h of annealing at 1000 degrees C in air. Along with the low thermal conductivity, the aliovalent ME perovskite can serve as a bifunctional shielding material for applications in aircraft engines and reusable rockets. A highly deficient medium-entropy perovskite ceramic has developed as an efficient electromagnetic interference shielding material in harsh environment. The high concentration of Ti-O vacancy clusters formed under the synergistic effect of aliovalent substitution and entropy effect enables the material to serve as an bifunctional shielding material for electromagnetic wave and heat. image
Keyword ：
aliovalent substitution aliovalent substitution electromagnetic interference shielding electromagnetic interference shielding harsh environment harsh environment medium-entropy ceramic medium-entropy ceramic vacancies vacancies
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| GB/T 7714 | Liu, Yongping , Tuo, Ping , Dai, Fu-Zhi et al. A Highly Deficient Medium-Entropy Perovskite Ceramic for Electromagnetic Interference Shielding under Harsh Environment [J]. | ADVANCED MATERIALS , 2024 , 36 (28) . |
| MLA | Liu, Yongping et al. "A Highly Deficient Medium-Entropy Perovskite Ceramic for Electromagnetic Interference Shielding under Harsh Environment" . | ADVANCED MATERIALS 36 . 28 (2024) . |
| APA | Liu, Yongping , Tuo, Ping , Dai, Fu-Zhi , Yu, Zhiyang , Lai, Wei , Ding, Qi et al. A Highly Deficient Medium-Entropy Perovskite Ceramic for Electromagnetic Interference Shielding under Harsh Environment . | ADVANCED MATERIALS , 2024 , 36 (28) . |
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The photoreduction of the CO2 reaction is a potential technique for converting solar energy to fuel at room temperature, which speeds up the recycling and conversion of carbon compounds. Based on a highly active photocatalyst, however, disentangling the chemical environments of surface structures on the selectivity of the product at the atomic scale is challenging. Herein, we have explored a sulfur-assisted heat treatment strategy to induce the reconstruction from surface-ordered line defects to polygonal tungsten line defects, changing the main product from CH4 (8.2 mu mol h(-1), 5 mg) to CO (13.0 mu mol h(-1), 5 mg) without any additive sacrificial agents. The experimental results reveal that the active sites are the surface terminations of the hexagonal-tungsten line defect, where the in-plane-neighboring W atoms can break the C-O bonds inside the *COOH intermediates, thereby promoting the desorption of CO gas.
Keyword ：
atomic level atomic level CO2 activation CO2 activation defect engineering defect engineering photocatalysis photocatalysis surface reconstruction surface reconstruction
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| GB/T 7714 | Shen, Min , Ye, Yan , Wang, Mingyue et al. Engineering the Atomic Configurations of Surface-Active Sites for Retuning the Photoreduction CO2 Selectivity [J]. | ACS CATALYSIS , 2024 , 14 (21) : 15908-15915 . |
| MLA | Shen, Min et al. "Engineering the Atomic Configurations of Surface-Active Sites for Retuning the Photoreduction CO2 Selectivity" . | ACS CATALYSIS 14 . 21 (2024) : 15908-15915 . |
| APA | Shen, Min , Ye, Yan , Wang, Mingyue , Liang, Xiaocong , Tang, Hao , Wang, Yulan et al. Engineering the Atomic Configurations of Surface-Active Sites for Retuning the Photoreduction CO2 Selectivity . | ACS CATALYSIS , 2024 , 14 (21) , 15908-15915 . |
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Adsorption and activation of C-H bonds by photocatalysts are crucial for the efficient conversion of C-H bonds to produce high-value chemicals. Nevertheless, the delivery of surface-active oxygen species for C-H bond oxygenation inevitably needs to overcome obstacles due to the separated active centers, which suppresses the catalytic efficiency. Herein, Ni dopants are introduced into a monolayer Bi2WO6 to create cascaded active units consisting of unsaturated W atoms and Bi/O frustrated Lewis pairs. Experimental characterizations and density functional theory calculations reveal that these special sites can establish an efficient and controllable C-H bond oxidation process. The activated oxygen species on unsaturated W are readily transferred to the Bi/O sites for C-H bond oxygenation. The catalyst with a Ni mass fraction of 1.8% exhibits excellent toluene conversion rates and high selectivity towards benzaldehyde. This study presents a fascinating strategy for toluene oxidation through the design of efficient cascaded active units.
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| GB/T 7714 | Shi, Yingzhang , Li, Peng , Chen, Huiling et al. Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers [J]. | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
| MLA | Shi, Yingzhang et al. "Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers" . | NATURE COMMUNICATIONS 15 . 1 (2024) . |
| APA | Shi, Yingzhang , Li, Peng , Chen, Huiling , Wang, Zhiwen , Song, Yujie , Tang, Yu et al. Photocatalytic toluene oxidation with nickel-mediated cascaded active units over Ni/Bi2WO6 monolayers . | NATURE COMMUNICATIONS , 2024 , 15 (1) . |
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Metal-organic frameworks (MOFs), characterized by tunable porosity, high surface area, and diverse chemical compositions, offer unique prospects for applications in optoelectronic devices. However, the prevailing research on thin-film devices utilizing MOFs has predominantly focused on aspects such as information storage and photosensitivity, often neglecting the integration of the advantages inherent in both photonics and electronics to enhance optical memory. This work demonstrates a light-mediated resistive memory device based on a highly oriented porphyrin-based MOFs film, in which the resistance state of the memristor is modulated by light, realizing the integration of the perception and storage of optical information. The memristor shows excellent performance with a wide light range of 405-785 nm and a persistent photoconductivity phenomenon up to 8.3 x 103 s. Further mechanistic studies have revealed that the resistive switching effect in the memristor is primarily associated with the reversible formation and annihilation of Ag conductive filaments. This work demonstrates a light-mediated resistive memory device based on a highly oriented porphyrin-based metal-organic frameworks film, in which the resistance state of the memristor is modulated by light, realizing the integration of the perception and storage of optical information. The memristor shows excellent performance with a wide light range of 405-785 nm and a persistent photoconductivity phenomenon up to 8.3 x 103 s. image
Keyword ：
film film metal-organic frameworks metal-organic frameworks optoelectronic memristors optoelectronic memristors porphyrins porphyrins resistance switching resistance switching
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| GB/T 7714 | Yang, Xue , Huang, Jian , Li, Jingjun et al. Optically Mediated Nonvolatile Resistive Memory Device Based on Metal-Organic Frameworks [J]. | ADVANCED MATERIALS , 2024 , 36 (35) . |
| MLA | Yang, Xue et al. "Optically Mediated Nonvolatile Resistive Memory Device Based on Metal-Organic Frameworks" . | ADVANCED MATERIALS 36 . 35 (2024) . |
| APA | Yang, Xue , Huang, Jian , Li, Jingjun , Zhao, Yanqi , Li, Hongfang , Yu, Zhiyang et al. Optically Mediated Nonvolatile Resistive Memory Device Based on Metal-Organic Frameworks . | ADVANCED MATERIALS , 2024 , 36 (35) . |
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Nanoconfined catalysts enhance stabilization of reaction intermediates, facilitate electron transfer, and safeguard active centers, leading to superior electrocatalytic activity, particularly in CO2 reduction reactions (CO2RR). Despite their effectiveness, crafting nanoconfined catalysts is challenging due to unclear formation mechanisms. In this study, we introduce an electrochemical method to grow Pd clusters within the interlayers of two-dimensional black phosphorus, creating Pd cluster-intercalated black phosphorus (Pd-i-BP) as an electrocatalyst. Using in situ electrochemical liquid phase transmission electron microscopy (EC-TEM), we revealed the synthesis mechanism of Pd-i-BP, involving electrochemically driven Pd ion intercalation followed by reduction within the BP layers. The Pd-i-BP electrocatalyst exhibits exemplary CO2-to-formate conversion, achieving 90% Faradaic efficiency for formate production, owing to its distinct nanoconfined structure that stabilizes intermediates and enhances electron transfer. Density functional theory (DFT) calculations underscore the structural benefits for enhancing intermediate adsorption and catalyzing the reaction. Our insights deepen understanding of nanoconfined material synthesis, promising advanced, high-efficiency catalysts.
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| GB/T 7714 | Xiao, Liangping , Zheng, Qizheng , Luo, Shiwen et al. Pd-intercalated black phosphorus: An efficient electrocatalyst for CO2 reduction [J]. | SCIENCE ADVANCES , 2024 , 10 (25) . |
| MLA | Xiao, Liangping et al. "Pd-intercalated black phosphorus: An efficient electrocatalyst for CO2 reduction" . | SCIENCE ADVANCES 10 . 25 (2024) . |
| APA | Xiao, Liangping , Zheng, Qizheng , Luo, Shiwen , Ying, Yifan , Zhou, Rusen , Zhou, Shiyuan et al. Pd-intercalated black phosphorus: An efficient electrocatalyst for CO2 reduction . | SCIENCE ADVANCES , 2024 , 10 (25) . |
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Owing to the large exciton binding energy(＞100 meV)of most organic materials,the process of exciton dissociation into free electrons and holes is seriously hindered,which plays a key role in the photocat-alytic system.In this study,a series of chalcogen(S,Se)-substituted mesoporous covalent organic frame-works(COFs)have been synthesized for enhanced photocatalytic organic transformations.Photoelectro-chemical measurements indicate that the introduction of semi-metallic Se atom and the enlargement of conjugation degree can not only reduce the exciton binding energy accelerating the charge separation,but also reduce the band gap of COFs.As a result,the COF-NUST-36 with the lowest exciton binding energy(39.5 meV)shows the highest photocatalytic performance for selective oxidation of amines(up to 98％Conv.and 97.5％Sel.).This work provides a feasible method for designing COFs with high photocatalytic activity by adjusting exciton binding energy.
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| GB/T 7714 | Zhangjie Gu , Zhen Shan , Yulan Wang et al. Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis [J]. | 中国化学快报（英文版） , 2024 , 35 (2) : 577-583 . |
| MLA | Zhangjie Gu et al. "Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis" . | 中国化学快报（英文版） 35 . 2 (2024) : 577-583 . |
| APA | Zhangjie Gu , Zhen Shan , Yulan Wang , Jinjian Wang , Tongtong Liu , Xiaoming Li et al. Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis . | 中国化学快报（英文版） , 2024 , 35 (2) , 577-583 . |
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