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2D MOF-assisted Pyrolysis-displacement-alloying Synthesis of High-entropy Alloy Nanoparticles Library for Efficient Electrocatalytic Hydrogen Oxidation
Authors:Ziming Qiu  Yong Li  Yidan Gao  Zhenyang Meng  Dr Yangyang Sun  Dr Yang Bai  Prof Nian-Tzu Suen  Prof Hsiao-Chien Chen  Dr Yecan Pi  Prof Huan Pang
Institution:1. School of Chemistry and Chemical Engineering, Yangzhou University, 225009 Yangzhou, Jiangsu, P.?R. China;2. School of Pharmacy, Changzhou University, 213164 Changzhou, Jiangsu, P.?R. China

State Key Laboratory of Coordination Chemistry, Nanjing University, 210023 Nanjing, Jiangsu, P.?R. China;3. Center for Reliability Science and Technologies, Chang Gung University, Kidney Research Center, Department of Nephrology, Chang Gung Memorial Hospital, Linkou, 333 Taoyuan, Taiwan

Abstract:Multimetallic alloy nanoparticles (NPs) have received considerable attention in various applications due to their compositional variability and exceptional properties. However, the complexity of both the general synthesis and structure–activity relationships remain the long-standing challenges in this field. Herein, we report a versatile 2D MOF-assisted pyrolysis-displacement-alloying route to successfully synthesize a series of binary, ternary and even high-entropy NPs that are uniformly dispersed on porous nitrogen-doped carbon nanosheets (PNC NSs). As a proof of utility, the obtained Co0.2Ru0.7Pt0.1/PNC NSs exhibits apparent hydrogen oxidation activity and durability with a record-high mass specific kinetic current of 1.84 A mg?1 at the overpotential of 50 mV, which is approximately 11.5 times higher than that of the Pt benchmark. Both experimental and theoretical studies reveal that the addition of Pt engenders a phase transition in CoRu alloys from hexagonal close-packed (hcp) to face-centered cubic (fcc) structure. The elevated reactivity of the resulted ternary alloy can be attributed to the optimized adsorption of hydrogen intermediate and the decreased reaction barrier for water formation. This study opens a new avenue for the development of highly efficient alloy NPs with various compositions and functions.
Keywords:Alloy Nanoparticles  Electrocatalysis  General Synthesis  Metal-Organic Framework Nanosheet  Ultrafine
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