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环境空气中单原子的闪光热冲击合成

Flash-Thermal Shock Synthesis of Single Atoms in Ambient Air.

作者信息

Kim Dong-Ha, Cha Jun-Hwe, Chong Sanggyu, Cho Su-Ho, Shin Hamin, Ahn Jaewan, Jeon Dogyeong, Kim Jihan, Choi Sung-Yool, Kim Il-Doo

机构信息

Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.

Membrane Innovation Center for Antivirus and Air-Quality Control, KAIST Institute Nanocentury, 291, Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea.

出版信息

ACS Nano. 2023 Dec 12;17(23):23347-23358. doi: 10.1021/acsnano.3c02968. Epub 2023 Oct 6.

Abstract

Single-atom catalysts feature interesting catalytic activity toward applications that rely on surface reactions such as electrochemical energy storage, catalysis, and gas sensors. However, conventional synthetic approaches for such catalysts require extended periods of high-temperature annealing in vacuum systems, limiting their throughput and increasing their production cost. Herein, we report an ultrafast flash-thermal shock (FTS)-induced annealing technique (temperature > 2850 °C, <10 ms duration, and ramping/cooling rates of ∼10 K/s) that operates in an ambient-air environment to prepare single-atom-stabilized N-doped graphene. Melamine is utilized as an N-doping source to provide thermodynamically favorable metal-nitrogen bonding sites, resulting in a uniform and high-density atomic distribution of single metal atoms. To demonstrate the practical utility of the single-atom-stabilized N-doped graphene produced by the FTS method, we showcased their chemiresistive gas sensing capabilities and electrocatalytic activities. Overall, the air-ambient, ultrafast, and versatile (e.g., Co, Ni, Pt, and Co-Ni dual metal) FTS method provides a general route for high-throughput, large area, and vacuum-free manufacturing of single-atom catalysts.

摘要

单原子催化剂对于依赖表面反应的应用(如电化学储能、催化和气体传感器)具有有趣的催化活性。然而,此类催化剂的传统合成方法需要在真空系统中进行长时间的高温退火,这限制了它们的产量并增加了生产成本。在此,我们报告了一种超快闪热冲击(FTS)诱导退火技术(温度>2850°C,持续时间<10毫秒,升温/降温速率约为10 K/s),该技术在环境空气环境中运行,用于制备单原子稳定的氮掺杂石墨烯。三聚氰胺用作氮掺杂源,以提供热力学上有利的金属 - 氮键合位点,从而导致单金属原子的均匀且高密度原子分布。为了证明通过FTS方法制备的单原子稳定氮掺杂石墨烯的实际效用,我们展示了它们的化学电阻式气体传感能力和电催化活性。总体而言,这种空气环境、超快且通用(例如钴、镍、铂和钴 - 镍双金属)的FTS方法为单原子催化剂的高通量、大面积和无真空制造提供了一条通用途径。

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