三维复合材料电极构筑及其能量存储与转化动力学的研究

With fast-growing demands for high-performance energy-storage and -conversion devices operating at low cost, there is considerable interest in developing novel electrode materials with enhanced electron and ion transport kinetics. This requires the electrode systems composing electroactive materials, conductive reinforcements and current collectors to possess the properties of large specific surface area, low internal resistance and high catalytic activity. In this proposal, facile synthesis technologies will be developed to prepare three-dimensional bicontinuous nanoporous hybrid materials and then seamlessly integrate them with current collectors for simultaneously addressing these requirements along the strategies of maximizing the specific surface area, minimizing the internal resistance and optimizing the catalytic activity. Special attention will be paid on the preparation and electrochemical properties of nanoporous metal-based composites and hybrids with unique crystallographic, interfacial and morphologic structures. During the course of the study, basic structure-activity relationships among their energy-storage and -conversion performances, microstructural properties and compositions will be demonstrated for the proposals of new principles and advanced designs of nanoporous hybrid electrodes with remarkably enhanced performance. Ultimately, the energy-storage and -conversion prototype devices will be constructed with these compositive electrode systems. Based on the implementation of this proposal, it is expected to deepen the understanding of physical mechanisms on the interactions and coupling effects in the metal-based heterostructures, and to achieve novel and high-performance materials, promoting the development of energy-storage and -conversion devices with high-energy and high-power densities as well as high efficiency.

以能量存储与转化器件低成本、高性能运行的需求为牵引，本项目拟以比表面积最大化、内阻最小化、催化性能最优化为实现途径，发展三维互连互通纳米多孔复合材料电极及其一体化集成的新方法和新原理，研发实用多孔金属复合材料的制备工艺；建立能量存储与转化服役性能与结构参数、成分之间的构效关系，最后获得高性能的储能与转化器件原型。实施本项目将有助于深入理解金属基异质结构相互作用的物理机制，为获得高比能、高比功率能量存储/输出和高效能量转化提供材料基础，推动燃料电池、超级电容等能量存储器件的商业化。

化石燃料过度消耗和排放所导致的严重环境污染影响着国民生活环境与经济的协调和可持续发展，促使着人类社会对绿色新能源的广泛需求。围绕能量存储与转化复合电极系统中电子输运/离子传输与扩散动力学、表面氧化还原反应动力学等关键科学问题，本项目顺利开展研究工作，取得了如下三方面主要进展：.(1).结合多体色散修正的密度泛函理论方法构建了金属材料/分子吸附体系的理论模型，系统研究了材料的结构及吸附性能，揭示了其表面吸附的机理，并建立了材料吸附与其本征性质的定量构效关系，为催化应用铺平了道路。.(2).揭示了甲酸催化放氢中Pd基合金催化剂的活性规律，建立了普适性的设计新策略；提出了高活性电催化合成氨催化材料设计原则，发展了电催化氮气还原合成氨的高性能Bi, Au及其复合物催化材料；提出了共晶结构模板法，研发了满足质传动力学、电子输运和高比表面积需求的多模式纳米多孔金属间化合物析氢和析氧反应、氧还原催化材料。.(3).提出了纳米多孔金属基复合电极材料一体化概念和导电介质/活性材料双相纳米结构化的设计思路，研发了系列新型纳米多孔金属/氧化物复合电极材料，构建了兼具高比能、高比功率和高稳定的(微型)能量存储器件；发展了相变驱动导电介质活化的新方法，发展了宽电压窗口的赝电容器；提出了共晶结构解决金属电池中金属负极材料因枝晶生长所引发的效率低、寿命短等问题，研发了高稳定、长寿命的锂钠、锌铝和铝铜合金电极材料，发展了高性能金属空气电池和水性金属电池。.自本项目运行以来，在Nat. Nanotechnol.，Nat. Chem.，Nat. Commun.，Sci. Adv.，Matter，Joule，Chem，Adv. Mater.等学术期刊共发表文章196篇，其中影响因子大于10的83篇，获得授权国家发明专利14件。以催化材料和纳米多孔金属材料为主题分别召开学术会议4次。20篇论文入选ESI高被引论文，其中7篇论文曾先后入选热点论文。项目负责人蒋青教授和项目成员鄢俊敏教授分别入选科睿唯安交叉学科领域“全球高被引科学家”；项目负责人蒋青教授在“全球顶尖前10万名科学家排名”中列4506名（中国排315名）；项目成员鄢俊敏获得国家杰出青年基金，郎兴友入选国家“万人计划”科技创新领军人才；王同辉和韩高峰分别入选2021年国家自然科学基金海外优秀青年基金；培养硕士/博士毕业研究生分别15/36人。

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