Zhang Huaifang, Ma Chaoqun, Wang Yi-Chi, Zhu Xiaojuan, Qu Kaiyu, Ma Xiao, He Caihong, Han Sumei, Liu Ai-Hua, Wang Qi, Cao Wenbin, Lin Wei, Xia Jing, Zhu Lijie, Gu Lin, Yun Qinbai, Wang An-Liang, Lu Qipeng
School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing, 100083, China.
Shunde Innovation School, University of Science and Technology Beijing, Foshan, 528399, China.
Angew Chem Int Ed Engl. 2024 Dec 2;63(49):e202409515. doi: 10.1002/anie.202409515. Epub 2024 Nov 6.
Gallium (Ga) with a low melting point can serve as a unique metallic solvent in the synthesis of intermetallic compounds (IMCs). The negative formation enthalpy of transition metal-Ga IMCs endows them with high catalytic stability. Meanwhile, their tunable crystal structures offer the possibility to tailor the configurations of active sites to meet the requirements for specific catalytic applications. Herein, we present a general method for preparing a range of transition metal-Ga IMCs, including Co-Ga, Ni-Ga, Pt-Ga, Pd-Ga, and Rh-Ga IMCs. The structurally ordered CoGa IMCs with body-centered cubic (bcc) structure are uniformly dispersed on the nitrogen-doped reduced graphene oxide substrate (O-CoGa/NG) and deliver outstanding nitrate reduction reaction (NORR) performance, making them excellent catalysts to construct highly efficient rechargeable Zn-NO battery. Operando studies and theoretical simulations demonstrate that the electron-rich environments around the Co atoms enhance the adsorption strength of *NO intermediate and simultaneously suppress the formation of hydrogen, thus improving the NORR activity and selectivity.
熔点较低的镓（Ga）可作为金属间化合物（IMC）合成中独特的金属溶剂。过渡金属 - 镓金属间化合物的负生成焓赋予它们高催化稳定性。同时，其可调谐的晶体结构为定制活性位点的构型提供了可能性，以满足特定催化应用的要求。在此，我们提出了一种制备一系列过渡金属 - 镓金属间化合物的通用方法，包括钴 - 镓、镍 - 镓、铂 - 镓、钯 - 镓和铑 - 镓金属间化合物。具有体心立方（bcc）结构的结构有序的钴镓金属间化合物均匀分散在氮掺杂还原氧化石墨烯基底上（O - CoGa/NG），并展现出出色的硝酸盐还原反应（NORR）性能，使其成为构建高效可充电锌 - 硝酸盐电池的优异催化剂。原位研究和理论模拟表明，钴原子周围富电子的环境增强了*NO中间体的吸附强度，同时抑制了氢的形成，从而提高了NORR活性和选择性。
