Physical and Materials Division, CSIR-National Chemical Laboratory, Pune 411 008, India; Academy of Scientific and Innovative Research, CSIR-Human Resource Development Centre (CSIR-HRDC) Campus, Postal Staff College area, Gaziabad 201 002, Uttar Pradesh, India.
Physical and Materials Division, CSIR-National Chemical Laboratory, Pune 411 008, India; Academy of Scientific and Innovative Research, CSIR-Human Resource Development Centre (CSIR-HRDC) Campus, Postal Staff College area, Gaziabad 201 002, Uttar Pradesh, India.
J Colloid Interface Sci. 2021 Oct 15;600:480-491. doi: 10.1016/j.jcis.2021.05.027. Epub 2021 May 11.
Efficient reduction of nitrogen to ammonia at a minimal cost would require a recherche catalyst tailored by assimilating the inherent electronic and reactive nature of Single Atom Catalysts (SACs) on heteroatom doped-graphene. A full-scale DFT study accounting for disparate descriptions of atomic orbitals and representation of support, has been carried out to identify the most active and recyclable SAC/B-graphene composite as catalyst for Nitrogen Reduction Reaction (NRR). Dual and Multiphilic descriptors derived reactivity pattern of six different metal SACs V, Fe, Ni, Ru, W and Re on periodic and non-periodic paradigms of pristine and BN-pair doped graphene supports, align with the calculated chemisorption efficacy and activation of N. The enzymatic route of nitrogen reduction on three most ideal metal SACs (V, W and Re) culminates Vanadium SAC, a relatively cheaper metal, anchored on BNring-graphene with an energy barrier of ⩽1.24 eV as a highly active and recyclable catalyst for NRR.
以最低成本将氮气高效还原为氨气，需要通过同化单原子催化剂（SAC）在杂原子掺杂石墨烯上固有的电子和反应性质，来定制一种研究深入的催化剂。这项研究进行了全面的密度泛函理论（DFT）研究，考虑了原子轨道的不同描述和支撑物的表示，以确定最活跃和可回收的 SAC/B-石墨烯复合材料作为氮还原反应（NRR）的催化剂。在周期性和非周期性的原始和 BN 对掺杂石墨烯支撑物模型上，六个不同金属 SACs（V、Fe、Ni、Ru、W 和 Re）的双亲和多亲描述符衍生的反应性模式与计算出的化学吸附效率和 N 的活化一致。三种最理想金属 SACs（V、W 和 Re）上的氮还原酶促途径以锚定在 BN 环石墨烯上的相对便宜的金属 V 结束，其能量势垒 ⩽1.24 eV，是一种高效且可回收的 NRR 催化剂。
