低配位铜基合金纳米片阵列的可控转化合成与硝酸根电还原合成铵性能

电催化水体中硝酸根污染物还原合成易回收的铵是一种“变废为宝”策略，得到了国内外同行的广泛关注。目前，铜基材料展现出较高的电催化性能，而且构筑低配位原子和合金结构可进一步提升其催化能力。但仍存在材料原子利用率低、低电位下活性和选择性较差、配位数与合金结构的作用机制和协同作用不清楚等问题。.本项目拟创新和发展电化学原位转化方法合成具有可控配位数和合金结构的CuM（M=Fe， Co，Ni，Zn等）纳米片阵列，通过二维纳米片结构提高材料的原子利用率，通过低配位结构和异质金属合金化协同调控Cu的电子密度，控制优化反应路径；采用多种原位谱学技术及理论模拟阐明催化过程中原子结构的动态演变及催化作用机制；构建流动式膜反应器，获得具有高时空产率的电催化反应装置。本项目将为探索低配位合金二维新材料的合成方法以及发展高效硝酸根电还原合成铵材料与装置提供科学依据。

Electrocatalytic reduction of nitrate pollutants in water to synthesize easily recycled ammonium is a strategy of "turning waste into treasure", and has attracted extensive attention from worldwide scholars. At present, the copper-based catalysts have shown promising performance, and the construction of low coordinate atoms and alloy structure can further improve the catalytic ability. However, the atom-utilization efficiency of these materials is still low, and the activity and selectivity are poor at low potential. Moreover, the mechanism and synergistic effect between coordination number and alloy structure are still unclear..Herein, we propose to develop novel in situ electrochemical conversion method to prepare CuM (M=Fe，Co，Ni，Zn, et al.) nanosheet arrays with controllable coordination number and alloy structure. Firstly, the atom-utilization efficiency of the material can be improved owing to the synthesis of two-dimensional nanosheets. Meanwhile, the electron density of Cu can be regulated collaboratively through low coordinate structure and alloying of heterogeneous metals, thus controlling and optimizing the reaction pathway. Secondly, combined with multiple in situ spectroscopy techniques and theoretical calculations, the dynamic evolution of the primary structure in the catalytic process and the mechanism of catalytic reaction will be revealed. Finally, the flow membrane reactor will be constructed to acquire the electrocatalytic reaction equipment with high space-time productivity. It is expected that our work will provide scientific guidance for the design of highly efficient electrocatalyst and reactor toward electroreduction of nitrate to ammonium.