Shear Field-Controlled Synthesis of Nitrogen-Doped Carbon Nanochains Forest with High-Density sp 3 Defects for Efficient CO 2 Electroreduction Reaction

作者：Xinyi Tan, Chang Yu, Yuanyang Xie, Zhao Wang, Lin Ni, Wenbin Li, Yafang Zhang, Song Cui, Jieshan Qiu · 发表于：ACS Nano · 年份：2024 · DOI：10.1021/acsnano.4c02591 · 被引用次数：15 · 研究领域：CO2 Reduction Techniques and Catalysts、Electrocatalysts for Energy Conversion、Electrochemical Analysis and Applications

Defect engineering and nitrogen doping being effective strategies for modulating the surface chemical state of the carbon matrix have been widely explored to promote the catalytic activity in the territory of electrochemical energy storage and conversion devices. However, the controllable synthesis of carbon material with high-density specific defects and high nitrogen doping is still full of challenges. Here, we first synthesize one-dimensional necklace-like nitrogen-doped carbon nanochains (N-CNCs) with abundant defects on carbon fiber paper (CFP) by chemical vapor deposition (CVD) method. The resultant nanostructures are a bunch of interconnected carbon spheres with a hollow structure at the internode and present the complete one-dimensional nanochain configuration. Specifically, the N-CNCs with a corrugated surface possesses high content of sp 3 defects (31.2%) and nitrogen (23.6 at %). Combining finite element analysis and experimental results, it reveals that the robust shear field generated by etching gas releasing from thermal decomposition of melamine in situ modulates the CVD process via changing the size and force environment of the metal catalyst droplets for formation of N-CNCs. Benefiting from the high ratio of sp 3 /sp 2 and nitrogen doped on the surface, the N-CNCs@CFP displays a superior electrocatalytic performance for CO 2 RR, delivering CO Faradaic efficiency of 95.9% and a current density of 23.2 mA cm –2 at −0.86 V vs RHE. This work provides promising sy...