A Non‐Equilibrium Flame Aerosol Process to Create High‐Entropy MOFs
Abstract
ABSTRACT High‐entropy alloys and ceramics have demonstrated promising applications in the past decade. Ultrafast heating and cooling can kinetically trap immiscible elements into solid solutions, expanding the compositional space and optimizing the properties of high‐entropy materials. However, the extreme temperatures required by these non‐equilibrium methods are incompatible with metal–organic frameworks (MOFs). This work presents a flame aerosol strategy for synthesizing compositionally complex, entropically stabilized MOFs, enabling new combinations of properties previously inaccessible in this class of materials. Using the HKUST structure as a prototype, this methodology is extended to a wide array of both crystalline and amorphous MOFs, and then to a 10‐element MOF that incorporates transition metals, rare‐earth metals, alkaline‐earth metals, p‐block metals, and noble metals. This strategy can be further applied to inorganic coordination polymers. This study reveals that kinetics and entropy collectively drive structural short‐range periodicity and configurational disorder in the framework, which in turn influence crystallinity, pore architecture, defect density, homogeneity, and electrochemical properties. This work expands the compositional design space for MOFs and offers new opportunities for their fundamental study and practical application.
Article Details
Authors (23)
Shuo Liu
Jiashun Liang
Department of Energy, Environmental & Chemical Engineering
Mohd Ashhar Khan
Shaon Das
Department of Materials Design and Innovation
Jialu Li
Chao Zheng
New Cornerstone Science Laboratory, State Key Laboratory of Organometallic Chemistry, Shanghai Institute of Organic Chemistry, University of Chinese Academy of Sciences, Chinese Academy of Sciences, 345 Lingling Lu, Shanghai 200032, China
Sanjit Ghose
National Synchrotron Light Source ∥, Brookhaven National Laboratory
Dominik Wierzbicki
National Synchrotron Light Source II
Qike Jiang
School of Engineering
Kaiwen Chen
Department of Chemical and Biological Engineering
Christina T. Scalzo
Department of Chemistry University at Buffalo The State University of New York Buffalo New York 14260 USA
Zhengxi Xuan
Department of Chemical and Biological Engineering
Sai Varun Karepakula
Department of Chemical and Biological Engineering University At Buffalo The State University of New York Buffalo New York USA
Yaoli Zhao
Department of Chemical and Biological Engineering University At Buffalo The State University of New York Buffalo New York USA
Kun Wang
Beijing National Laboratory for Molecular Science, State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering
Jinghua Guo
Baishakhi Mazumder
Department of Materials Design and Innovation
Wei Chen
Kaihang Shi
Gang Wu
Jeffrey J. Urban
Lawrence Berkeley National Laboratory
Mark T. Swihart
Department of Chemical and Biological Engineering
Chaochao Dun
The Molecular Foundry