Enthalpy-change driven synthesis of high-entropy perovskite nanoparticles
作者机构：School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China
出 版 物：《Nano Research》 (纳米研究（英文版）)
年 卷 期：2022年第15卷第6期
页 面：4867-4872页
核心收录：
学科分类：0808[工学-电气工程] 0809[工学-电子科学与技术（可授工学、理学学位）] 08[工学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0702[理学-物理学]
基 金：supported by National Natural Science Foundation of China(No.21776174) the National Key R&D Plan(No.2020YFB0606400) Shanghai Rising-Star Program(No.20QA1405200) Shanghai Jiao Tong University Scientific and Technological Innovation Funds(No.2019QYB06) China Shipbuilding Industry Corporation(CSIC)and Inner Mongolia Erdos Group.
主 题：enthalpy-change high-entropy ceramics mechanochemical synthesis perovskite CO oxidation
摘 要：Due to their diverse and tunable composition,distorted lattice and excellent stability,high-entropy ceramics(HECs)hold great promise for catalysis,especially when they present as nanoparticles(NPs).However,current HECs are typically limited to bulky materials with none or fewer defects,because high synthetic temperature(e.g.,1,000–1,200°C)is usually required to highlight the entropic contribution(TΔS)inΔG=ΔH−TΔS.Being different with previous strategies,a negative Gibbs free energy for HECs crystallization is obtained by dramatically decreasing the mixing enthalpy(ΔH).Guided by this principle,single-phase highentropy La(Ni_(0.2)Mn_(0.2)Cu_(0.2)Fe_(0.2)Co_(0.2))O_(3−δ)perovskite(HE-LMO)NPs were prepared at a relatively low temperature(≤500°C).Interestingly,abundant oxygen vacancies were directly created within HE-LMO NPs,which exhibited good activity in catalytic oxidation.Meanwhile,the high-entropy structure endows as-made HE-LMO with robust stability even with 5 vol.%water in feeding gas.Density functional theory(DFT)calculations revealed that the defective sites in HE-LMO NPs facilitated the charge transfer from HE-LMO to CO,thus activating the adsorbed CO gas.The current work may inspire future design and synthesis of HECs NPs.
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