Dual-metal-driven Selective Pathway of Nitrogen Reduction in Orderly Atomic-hybridized Re2MnS6 Ultrathin Nanosheets
Dual-metal-driven Selective Pathway of Nitrogen Reduction in Orderly Atomic-hybridized Re2MnS6 Ultrathin Nanosheets
复制标题
双金属驱动的有序原子杂化Re2MnS6超薄纳米片中氮还原的选择性途径
DOI：
10.1021/acs.nanolett.0c01037
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发表时间：
2020-07-08
期刊：
影响因子：
10.8
通讯作者：
Wu, Xinglong
中科院分区：
文献类型：
--
作者：
Fu, Yao;Li, Tinghui;Wu, Xinglong
可持续肥料和无碳能源载体的未来需要在开发高效电催化剂方面取得创新突破，以便在温和条件下从氮气（N-2）合成氨（NH3）。通过仔细的催化剂设计来理解和调节在催化剂表面上形成的反应中间体可以绕过与模糊的吸附物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Re 2 MnS 6纳米片，其中包括有序杂化Mn-Re双金属网站通过强Hubbard电子-电子相互作用，展示了一个有前途的选择性对反应过程从N-2到NH3。Mn位的有序包含导致结构相变和非键合半金属状态的出现，其中限速活化能势垒通过反应途径中的转化而显著降低。结果表明，与单一金属ReS 2相比，Re 2 MnS 6的N-2还原性能提高了约6.6倍。
The future of sustainable fertilizers and carbon-free energy carrier demands innovative breakthroughs in the exploitation of efficient electrocatalysts for synthesizing ammonia (NH3) from nitrogen (N-2) 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 Re2MnS6 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-2 to NH3. 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-2 reduction in Re2MnS6 is increased about 6.6 times compared to the single-metal ReS2.