过电位
析氧
材料科学
催化作用
电子转移
密度泛函理论
聚合物
合理设计
化学工程
X射线吸收光谱法
纳米技术
薄膜
物理化学
吸收光谱法
计算化学
化学
有机化学
电化学
电极
复合材料
工程类
物理
量子力学
作者
Yonggui Zhao,Wenchao Wan,Yi Chen,Rolf Erni,Carlos A. Triana,Jingguo Li,Christos K. Mavrokefalos,Ying Zhou,Greta R. Patzke
标识
DOI:10.1002/aenm.202002228
摘要
Abstract Engineering low‐crystalline and ultra‐thin nanostructures into coordination polymer assemblies is a promising strategy to design efficient electrocatalysts for energy conversion and storage. However, the rational utilization of coordination polymers (CPs) or their derivatives as electrocatalysts has been hindered by a lack of insight into their underlying catalytic mechanisms. Herein, a convenient approach is presented where a series of Ni 10‐x Fe x ‐CPs (0 ≤ x ≤ 5) is first synthesized, followed by the introduction of abundant structural deficiencies using a facile reductive method (R‐Ni 10‐x Fe x ‐CPs). The representative low‐crystalline R‐Ni 8 Fe 2 ‐CPs (R‐NiFe‐CPs) with a thickness of sub‐2 nm display promising oxygen evolution reaction (OER) performance with a very low overpotential of 225 mV at 10 mA cm −2 and high long‐term durability over 120 h. Comprehensive investigations including X‐ray absorption spectroscopy, density functional theory, and mass diffusion theory reveal strong synergistic effects of structural deficiencies on the OER activity. A super‐Nernstian pH‐dependence of 85.15 mV pH −1 suggests that the catalytic OER mechanism of R‐NiFe‐CPs involved a decoupled proton‐electron transfer (PT/ET) pathway, leading to notably higher OER activity compared to the concerted coupled proton‐electron transfer pathway. New insights into the catalytic reaction mechanisms of CP‐related materials open up new approaches to expedite the design of efficient electrocatalysts.
科研通智能强力驱动
Strongly Powered by AbleSci AI