北京理工大学陈文星团队利用原子印刷策略实现了双铜原子在C2N结构上的精确锚定,有效地将CO2还原为乙烯。相关研究成果发表在2024年9月9日出版的《德国应用化学》。
孤立金属位点催化剂(IMSCs)在电化学CO2还原中起着至关重要的作用,具有潜在的工业应用前景。然而,IMSCs的可调合成策略是有限的。
该文中,研究人员提出了一种原子印刷策略,其灵感来自中国古代的“活字印刷技术”。选择可定制的金属原子组合作为金属前体,形成一个广泛的双核金属库。通过利用C2N腔中的边缘氮原子作为锚定“钳子”来捕获金属原子,制备了一系列双原子催化剂。
为了证明其实用性,研究了双原子催化剂Cu2-C2N作为电催化CO2RR催化剂。双Cu原子的协同作用促进了C-C耦合,并保证了FEC2+(90.8%)和FEC2H4。与RHE相比,-1.10 V时为71.7%。DFT计算表明,在CO2RR过程中,Cu2位点会发生微妙的翻转,以增强*CO的吸附和二聚。
研究人员验证了原子打印策略适用于广泛的金属组合,代表了IMSC发展的重大进步。
附:英文原文
Title: Atomic Printing Strategy Achieves Precise Anchoring of Dual-Copper Atoms on C2N Structure for Efficient CO2 Reduction to Ethylene
Author: Zhiyi Sun, Xuan Luo, Huishan Shang, Ziding Wang, Liang Zhang, Wenxing Chen
Issue&Volume: 2024-09-09
Abstract: Isolated metal sites catalysts (IMSCs) play crucial role in electrochemical CO2 reduction, with potential industrial applications. However, tunable synthesis strategies for IMSCs are limited. Herein, we present an atomic printing strategy that draws inspiration from the ancient Chinese "movable-type printing technology". Selecting customizable combinations of metal atoms as metal precursors form an extensive binuclear metal library. A series of dual-atom catalysts were prepared by utilizing the edge nitrogen atoms in the C2N cavity as anchoring "pincers" to capture metal atoms. To prove utility, the dual atom catalyst Cu2-C2N is investigated as electrocatalytic CO2RR catalyst. The synergistic interaction of dual Cu atoms promotes C-C coupling and guarantees FEC2+ (90.8%) and FEC2H4. (71.7%) at -1.10 V vs RHE. DFT calculations revealed the Cu2 site would be subtly flipped during CO2RR for enhancing *CO adsorption and dimerization. We validate that atomic printing strategies are applicable to wide range of metal combinations, representing a significant advancement in the development of IMSCs.
DOI: 10.1002/anie.202405778
Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202405778
Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx