C2N-supported single metal ion catalysts for HCOOH dehydrogenation
C2N-supported single metal ion catalysts for HCOOH dehydrogenation
复制标题
C2N负载单金属离子HCOOH脱氢催化剂
DOI：
10.1039/c8ta02299b
复制
发表时间：
2018
影响因子：
11.9
通讯作者：
Jiang Jun
中科院分区：
文献类型：
--
作者：
Zhong Wenhui;Liu Yuxia;Deng Mingsen;Zhang Yachao;Jia Chuanyi;Prezhdo Oleg V.;Yuan Jianyong;Jiang Jun
在二维C2 N晶格上锚定的单原子过渡金属离子（TMx+）对HCOOH脱氢具有高催化性能。考虑到Co2+，Cu 2+和Ni 2+的非贵金属离子负载C2 N，我们使用密度泛函理论证明脱氢的能量势垒低的纯Pt和Pd催化剂。高的催化性能归因于反应通过TMx+和邻近的C2 N的N原子组成的双活性中心进行。具体而言，C2 N-Co2+在低自旋状态（S = 1/2），大大促进HCOOH脱氢的速度决定步骤的势垒降低到只有0.30 eV，主要是由于TMx+的强大能力，以提取电荷从HCOOH和C2 N。所获得的机理的见解有助于合理设计的单原子基过渡金属离子催化剂的二维材料支持。
High catalytic performance of a single-atom transition metal ion (TMx+) anchored on the two-dimensional (2D) C2N lattice is predicted for HCOOH dehydrogenation. Considering the Co2+, Cu2+ and Ni2+ non-noble metal ions supported by C2N, we use density functional theory to demonstrate dehydrogenation energy barriers as low as those for pure Pt and Pd catalysts. The high catalytic performance is ascribed to the reaction occurring through a dual-active center composed of TMx+ and a nearby N atom of C2N. Specifically, C2N–Co2+ in the low spin state (S = 1/2) greatly promotes HCOOH dehydrogenation by decreasing the barrier of the rate-determining step to only 0.30 eV, mainly due to the strong ability of TMx+ to extract charges from HCOOH and C2N. The obtained mechanistic insights help the rational design of single-atom based transition metal ion catalysts supported by 2D materials.