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Electrochemical Oxidative Dehydrogenation of Ethane to Ethylene in a Solid Oxide Electrolyzer

Angewandte Chemie 2021年第40期133卷

作者： Lingting Ye Xiuyun Duan Prof. Dr. Kui Xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Key Laboratory of Design & Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou Guangdong 116023 China

Oxidative dehydrogenation of ethane to ethylene is an important process in light olefin industry; however, the over-oxidation of ethane leads to low ethylene selectivity. Here, we report a novel approach to electrochemical oxidative dehydrogenation of ethane in anode in conjunction with CO 2 reduction at cathode in a solid oxide electrolyser using a porous single-crystalline CeO 2 electrode at 600 °C. We identify and engineer the flux and chemical states of active oxygen species that evolve from the lattice at anode surface to activate and dehydrogenate ethane to ethylene via the reaction of epoxy species. Active oxygen species (O 2− , O 2 2− and O 2 − ) at the anode surface effectively dehydrogenate ethane to ethylene, but O − species tend to induce deep oxidation. We demonstrate exceptionally high ethylene selectivity of 95 % and an ethane conversion of 10 % with a durable operation of 300 h.

关键词： active oxygen species electrochemical oxidative dehydrogenation ethane porous single crystals solid oxide electrolyzer

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A novel multi-scale continuum electric double-layer model for electron-proton interplay at the TiO2/electrolyte interface

A novel multi-scale continuum electric double-layer model fo...

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中国化学会第二十次全国电化学大会

作者： Jie-qiong Li Lingyi Meng Jun Cheng State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials College of Chemistry and Chemical Engineering Xiamen University CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences Xiamen Institute of Rare-earth Materials Haixi Institutes Chinese Academy of Sciences

Although photoelectrochemical water oxidation has received considerable theoretical and experimental investigations[1,2], there is still a lack of studies involving the interaction between electric field and charge at the semiconductor/electrolyte interface. This interaction is crucial to determine the interfacial behaviors of photoelectrochemistry.

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Cooperative Catalysis of Polysulfides in Lithium-Sulfur Batteries through Adsorption Competition by Tuning Cationic Geometric Configuration of Dual-active Sites in Spinel Oxides

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Angewandte Chemie 2022年第8期135卷

作者： Dr. Hongtai Li Pei Shi Lei Wang Tianran Yan Tong Guo Xiao Xia Prof. Chi Chen Prof. Jing Mao Prof. Dan Sun Prof. Liang Zhang Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou 215123 China Contribution: Conceptualization (lead) Formal analysis (lead) Writing - original draft (lead) CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen 361021 China Contribution: Data curation (lead) Investigation (equal) Contribution: Investigation (equal) Validation (equal) Contribution: Investigation (equal) Key Laboratory for Soft Chemistry and Functional Materials of Ministry of Education Nanjing University of Science and Technology Nanjing 210094 China Contribution: Data curation (equal) Investigation (equal) School of Materials Science and Engineering Zhengzhou University Zhengzhou 450001 China Contribution: Investigation (equal) Supervision (equal) Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China Contribution: Conceptualization (lead) Funding acquisition (lead) Supervision (lead) Writing - review & editing (lead)

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Intramolecular Noncovalent Interaction-Enabled Dopant-Free Hole-Transporting Materials for High-Performance Inverted Perovskite Solar Cells

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Angewandte Chemie 2021年第2期134卷

作者： Dr. Kun Yang Qiaogan Liao Dr. Jun Huang Zilong Zhang Mengyao Su Dr. Zhicai Chen Ziang Wu Dong Wang Ziwei Lai Prof. Han Young Woo Prof. Yan Cao Prof. Peng Gao Prof. Xugang Guo Department of Materials Science and Engineering Guangdong Provincial Key Laboratory of Functional Oxide Materials and Devices Southern University of Science and Technology (SUSTech) No. 1088 Xueyuan Road Shenzhen Guangdong 518055 China School of Materials Science and Engineering Harbin Institute of Technology Harbin 150001 China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Provincial Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Department of Chemistry Korea University Seoul 136–713 Republic of Korea Institute of Advanced Study Shenzhen University Shenzhen Guangdong 518060 China

Intramolecular noncovalent interactions (INIs) have served as a powerful strategy for accessing organic semiconductors with enhanced charge transport properties. Herein, we apply the INI strategy for developing dopant-free hole-transporting materials (HTMs) by constructing two small-molecular HTMs featuring an INI-integrated backbone for high-performance perovskite solar cells (PVSCs). Upon incorporating noncovalent S⋅⋅⋅O interaction into their simple-structured backbones, the resulting HTMs, BTORA and BTORCNA, showed self-planarized backbones, tuned energy levels, enhanced thermal properties, appropriate film morphology, and effective defect passivation. More importantly, the high film crystallinity enables the materials with substantial hole mobilities, thus rendering them as promising dopant-free HTMs. Consequently, the BTORCNA-based inverted PVSCs delivered a power conversion efficiency of 21.10 % with encouraging long-term device stability, outperforming the devices based on BTRA without S⋅⋅⋅O interaction (18.40 %). This work offers a practical approach to designing charge transporting layers with high intrinsic mobilities for high-performance PVSCs.

关键词： dopant-free hole-transporting materials hole mobility noncovalent interactions perovskites solar cells

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MATGANIP: Learning to Discover the Structure-Property Relationship in Perovskites with Generative Adversarial Networks

arXiv

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arXiv 2019年

作者： Hu, Junjie Li, Mu Gao, Peng CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences FuzhouFujian350002 China Institute of Software Chinese Academy of Sciences Beijing100190 China Laboratory of Advanced Functional Materials Xiamen Institute of Rare Earth Materials Haixi Institute Chinese Academy of Sciences Xiamen361021 China University of Chinese Academy of Sciences Beijing100049 China

Accelerating the design of materials with artificial neural network draws more attention due to its magnitude potential. In the past works, some tools of materials information have been developed to promote the industrialize of state-of-the-art materials, such as the materials project, AFlow, and open quantum materials database. Else, more various endeavors are required for artificial general intelligence in the area of materials. In our works, we design neural networks named MATGANIP, which applies a combination of generative adversarial networks, graph networks, convolutional neural networks, and long short term memory for the perovskite materials. We adopt it for the building of a structure-property relationship, where the trained properties contain: the computational geometric property, tolerance factor;and the ground state property of Quantum theory, the vacuum energy. Moreover, the data-set about the ABX3 perovskites is used for the learning of tolerance factor, to extend its function of tolerance factor into the structural identification of the arrangement of disorder atoms;another data-set about the density functional theory (DFT) calculation results is for the ground state energy of quantum theory, to obtain the more accurate result than the training of DFT calculated results in similar works. In our training task of the DFT date-set, we adopt the intuitive criterion to evaluate its performance: the mean absolute error (MAE) is smaller than 0.3 meV/atom, and the mean absolute error rate (MAER) is smaller than 0.01%. These results prove the potential ability of our MATGANIP in developing the relationship between materials structure and their properties. Notably, it suits for some scenes involved massive possible structures and their properties, such as the arrangement of the atoms in the structural phase transition of the inorganic perovskites with mixed atoms. Copyright © 2019, The Authors. All rights reserved.

关键词： Density functional theory

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Active Exsolved Metal–Oxide Interfaces in Porous Single-Crystalline Ceria Monoliths for Efficient and Durable CH4/CO2Reforming

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Angewandte Chemie 2021年第1期134卷

作者： Yongchun Xiao Prof. Kui Xie Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Key Laboratory of Design & Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou Guangdong 116023 China University of Chinese Academy of Sciences Beijing 100049 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China

Dry reforming of CH 4 /CO 2 provides an attractive route to convert greenhouse gas into syngas; however, the resistance to sintering and coking of catalyst remains a fundamental challenge at high operation temperatures. Here we create active and durable metal–oxide interfaces in porous single-crystalline (PSC) CeO 2 monoliths with in situ exsolved single-crystalline (SC) Ni particles and show efficient dry reforming of CH 4 /CO 2 at temperatures as low as 450 °C. We show the excellent and durable performance with ≈20 % of CH 4 conversion and ≈30 % of CO 2 conversion even in a continuous operation of 240 hours. The well-defined active metal–oxide interfaces, created by exsolving SC Ni nanoparticles from PSC Ni x Ce 1− x O 2 to anchor them on PSC CeO 2 scaffolds, prevent nanoparticle sintering and enhance the coking resistance due to the stronger metal–support interactions. Our work would enable an industrially and economically viable path for carbon reclamation, and the technique of creating active and durable metal–oxide interfaces in PSC monoliths could lead to stable catalyst designs for many challenging reactions.

关键词： ceria dry reforming exsolution metal–oxide interfaces porous single crystals

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Enhanced photostability and targeting ability of hollow mesoporous manganese-based nanocarriers for NIR-II fluorescence image-guided surgery and photothermal therapy

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Journal of colloid and interface science 2025年 698卷 138094页

作者： Yu Ye Xiangchen Zeng Zhong Luo Wenxuan Gan Yongying Dang Shuoqi Yang Yuxiang Zhang Xingfeng Qiu Tong Zhang Zhenshuang Du Peiyuan Wang Weiling He Department of Gastrointestinal Surgery Xiang'an Hospital of Xiamen University School of Medicine Xiamen University Xiamen Fujian 361000 China. State Key Laboratory of Molecular Vaccinology and Molecular Diagnostics School of Public Health Xiamen University Xiamen Fujian 361000 China. Organ Transplantation Clinical Medical Center of Xiamen University Department of General Surgery Xiang'an Hospital of Xiamen University School of Medicine Xiamen University Xiamen 361102 China. Electronic address: zhangtong@***. Department of General Practice Xiang'an Hospital of Xiamen University School of Medicine Xiamen University Xiamen Fujian 361000 China. Electronic address: zsdu@***. Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China. Electronic address: wangpeiyuan@***. Department of Gastrointestinal Surgery Xiang'an Hospital of Xiamen University School of Medicine Xiamen University Xiamen Fujian 361000 China Department of Gastrointestinal Surgery The First Affiliated Hospital Sun Yat-sen University Guangzhou Guangdong 510080 China. Electronic address: wlhe@***.

Hollow mesoporous manganese (HMM)-based nanocarriers, incorporating nanoparticle cavities and mesoporous channels, enhance the photostability and photobleaching resistance of indocyanine green (ICG). The addition of H2N-c(RGDfK)-OH (RGD) ensures precise targeting, making the cRGD&PEG2000-HMM@ICG (R&P-M@ICG) nanoprobe ideal for NIR-II fluorescence image-guided surgery and photothermal therapy (PTT). This approach offers accurate targeting, high therapeutic efficacy, and reduced side effects. The inclusion of manganese (Mn) in the nanocarriers further boosts the therapeutic effects by enabling chemodynamic therapy (CDT). Mn ions catalyze the conversion of hydrogen peroxide (HO) into highly reactive hydroxyl radicals (•OH) within the tumor microenvironment. The synergy between Mn-driven CDT and PTT enhances tumor ablation, as the heat from PTT accelerates ROS production from CDT, leading to more effective tumor cell damage and apoptosis. The dual action of PTT and CDT overcomes the limitations of single-modal therapies. While PTT induces hyperthermia to kill tumor cells, Mn-assisted CDT amplifies the ROS generation, further enhancing treatment efficacy. This combined effect makes the R&P-M@ICG nanoprobe a powerful tool for cancer treatment, demonstrating superior anti-tumor efficacy compared to conventional therapies. In this study, we synthesized the R&P-M@ICG nanoprobe, highlighting its potential for precise surgical navigation, and for synergistic photothermal and chemodynamic therapy in cancer treatment.

关键词： Colorectal cancer Hollow mesoporous manganese Indocyanine green NIR-II imaging Photothermal therapy

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Kinetic Control of Hexagonal Mg（OH）2 Nanoflakes for Catalytic Application of Preferential CO Oxidation

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Chinese Journal of Chemistry 2017年第6期35卷 903-910页

作者： Huixia Li Liping Li Shaoqing Chen Yuelan Zhang Guangshe Li State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 China Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Fuzhou Fujian 350002 China

Controlling the growth of nanocrystals is one of the most challenged issues in current catalytic field, which helps to further understand the size and morphology related behaviors for catalytic applications. In this work, we investigated the plane growth kinetics of Mg（OH）2 for catalytic application in preferential CO oxidation. Nanoflakes were synthesized through hydrothermal method. The morphology and structure of nanoflakes were characterized by TEM, SEM, and XRD. By varying the reaction temperature and time, Mg（OH）2 nanoflakes un- derwent an anisotropic growth. Benefited from the Ostwald ripening process, the thickness of nanoflake corre- sponding to the （110） plane of Mg（OH）2 was tuned from 7.6 nm to 24.0 nm, while the diameter of （001） plane in- creased from 18.2 nm to 30.2 nm. The grain growth kinetics for the thickness was well described in terms of an equation, D5= 7.65＋ 6.9 × 10^8exp（-28.14/RT）. After depositing Pt nanoparticles onto these Mg（OH）2 nanoflakes, an excellent catalytic performance was achieved for preferential CO oxidation in H2-rich streams with a wide temper- ature window from 140 ℃ to 240 ℃ for complete CO conversion due to the interaction between Pt and hydroxyl groups. The findings reported here would be helpful in discovering novel catalysts for application of proton ex- change membrane fuel cells.

关键词： kinetics CO-PROX size-dependent nanoflakes

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Pr3+/Yb3+:NaGdF4@ Yb3+:NaYF4 Core/ Shell Nanocrystals: Synthesis, Microstructure and Quantum-Cutting Luminescence

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Microscopy and Microanalysis 2018年第S1期24卷 1724-1725页

作者： Yuansheng Wang CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002(P. R. China)

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Simultaneous removal of Cu(Ⅱ) and Cr(Ⅵ) by Mg–Al–Cl layered double hydroxide and mechanism insight

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Journal of Environmental Sciences 2017年第3期29卷 16-26页

作者： Xianyang Yue Weizhen Liu Zuliang Chen Zhang Lin Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of Sciences School of Environment and Energy South China University of Technology Centre for Environmental Risk Assessment and Remediation University of South Australia

Mg-A1-C1 layered double hydroxide （C1-LDH） was prepared to simultaneously remove Cu（II） and Cr（VI） from aqueous solution. The coexisting Cu（II）（20 mg/L） and Cr（VI）（40 mg/L） were completely removed within 30 min by C1-LDH in a dosage of 2.0 g/L; the removal rate of Cu（II） was accelerated in the presence of cr（VI）. Moreover, compared with the adsorption of single Cu（II） or Cr（VI）, the adsorption capacities of C1-LDH for Cu（II） and Cr（VI） can be improved by 81.05% and 49.56%, respectively, in the case of coexisting Cu（II）（200 mg/L） and Cr（VI）（400 mg/L）. The affecting factors （such as solution initial pH, adsorbent dosage, and contact time） have been systematically investigated. Besides, the changes of pH values and the concentrations of Mg2＋ and A13＋ in relevant solutions were monitored. To get the underlying mechanism, the C1-LDH samples before and after adsorption were thoroughly characterized by X-ray powder diffraction, transmission electron microscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. On the basis of these analyses, a possible mechanism was proposed. The coadsorption process involves anion exchange of Cr（VI） with C1- in C1-LDH interlayer, isomorphic substitution of Mg2＋ with Cu2＋, formation of Cu2CI（OH）3 precipitation, and the adsorption of Cr（VI） by Cu2CI（OH）3. This work provides a new insight into simultaneous removal of heavy metal cations and anions from wastewater by CI-LDH.

关键词： AdsorptionHeavy metalsLayered double hydroxideAnion exchangePrecipitation

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