Fu Yao, Li Tinghui, Zhou Gang, Guo Junhong, Ao Yanhui, Hu Youyou, Shen Jiancang, Liu Lizhe, Wu Xinglong
Key Laboratory of Modern Acoustics, MOE, Institute of Acoustics and Collaborative Innovation Center of Advanced Microstructures, National Laboratory of Solid State Microstructures, Nanjing University, Nanjing 210093, People's Republic of China.
College of Electronic Engineering, Guangxi Normal University, Guilin 541004, People's Republic of China.
Nano Lett. 2020 Jul 8;20(7):4960-4967. doi: 10.1021/acs.nanolett.0c01037. Epub 2020 Jun 2.
The future of sustainable fertilizers and carbon-free energy carrier demands innovative breakthroughs in the exploitation of efficient electrocatalysts for synthesizing ammonia (NH) from nitrogen (N) in mild conditions. Understanding and regulating the reaction intermediates that form on the catalyst surface through careful catalyst design could bypass certain limitations associated with ambiguous adsorbate evolution mechanism. Herein, we propose ternary intermetallic ReMnS ultrathin nanosheets that include orderly hybridized Mn-Re dual-metal sites through strong Hubbard e-e interaction, demonstrating a promising selectivity toward reaction process from N to NH. The ordered inclusion of Mn sites leads to a structural phase transition and appearance of nonbonding semimetal states, in which the rate-limiting activation energy barrier is significantly decreased through a conversion in reaction pathway. As a result, the performance of N reduction in ReMnS is increased about 6.6 times compared to the single-metal ReS.
可持续肥料和无碳能源载体的未来需要在温和条件下从氮气（N）合成氨（NH₃）的高效电催化剂开发方面取得创新性突破。通过精心设计催化剂来理解和调控在催化剂表面形成的反应中间体，可以绕过与模糊的吸附质演化机制相关的某些限制。在此，我们提出了三元金属间化合物ReMnS超薄纳米片，其通过强哈伯德电子-电子相互作用包含有序杂交的Mn-Re双金属位点，对从N到NH₃的反应过程表现出有前景的选择性。Mn位点的有序包含导致结构相变和非键合半金属态的出现，其中通过反应路径的转变显著降低了限速活化能垒。结果，与单金属ReS相比，ReMnS中N还原的性能提高了约6.6倍。
