Electrochemical nitrogen reduction reaction on anchored SnS2 nanosheets with TM2 dimers.
Electrochemical nitrogen reduction reaction on anchored SnS2 nanosheets with TM2 dimers.
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DOI：
10.1016/j.jcis.2024.01.081
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发表时间：
2024-01
影响因子：
9.9
通讯作者：
Ruixin Xu;Shiqian Cao;Tingting Bo;Nan Mu;Yanyu Liu;Wei Zhou
中科院分区：
文献类型：
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作者：
Ruixin Xu;Shiqian Cao;Tingting Bo;Nan Mu;Yanyu Liu;Wei Zhou
设计高效、高稳定性的固氮催化剂是实现环境条件下电化学氮还原反应的一大挑战。本文通过高通量第一性原理计算，从固定在sns2纳米片上的过渡金属（TM）二聚体中获得了潜在的电化学NRR催化剂。所选W2/ sns2具有- 0.27 V的极限势和0.81 eV的最大动力学势，表现出* n2相对于其他小分子（*H2O、*O、*OH、*H）的吸附优势。更重要的是，减慢TM原子的轨道价电子数和电负性可以获得更好的NRR活性，并提出了一种考虑配位环境和吸附剂影响的新描述子φ，实现了对各种候选物的快速预筛选。这项工作为快速筛选TM2/ sns2候选物以实现高效固氮和进一步简化电化学NRR催化剂的设计提供了实用的见解。
The design of efficient, high-stability nitrogen fixation catalysts remains a great challenge to achieve electrochemical nitrogen reduction reaction (NRR) under ambient conditions. Herein, the high-throughput first-principles calculations are performed to obtain potential electrochemical NRR catalysts from transition metal (TM) dimers anchored on SnS2nanosheets. The selected W2/SnS2behaves as a promising NRR candidate possessing −0.27 V limiting potential and 0.81 eV maximum kinetic potential, and it exhibits the adsorption advantages of *N2over other small molecules (*H2O, *O, *OH, *H). More importantly, the moderatedorbital valence electron number and electronegativity of TM atom could obtain better NRR activity, and a new descriptorφconsidering the effects of coordination environments and adsorbates is proposed to achieve the fast pre-screening among various candidates. This work presents practical insights into the fast screening of TM2/SnS2candidates for efficient nitrogen fixation and further streamlining the design of electrochemical NRR catalysts.