Role of bonding filling on HER/OER/ORR multifunctional catalytic activity in transition-metals-doped PdPX(X=S,Se,Te)  

作　　者：Hai-Hua Huang Wei Li Cheng-Chao Hu Xue-Qin Sun Lin-Guo Lu Xiao-Feng Fan 

机构地区：[1]School of Materials Science and Engineering,Laboratory of Sensitive Materials and Devices,Shandong Department of Education,Liaocheng University,Liaocheng 252059,China [2]School of Environmental and Material Engineering,Yantai University,Yantai 264005,China [3]Department of Physics,University of Puerto Rico,Rio Piedras,San Juan.PR00931,USA [4]Key Laboratory of Automobile Materials(Jilin University),Ministry of Education,College of Materials Science and Engineering,Jilin University,Changchun 130012,China

出　　处：《Rare Metals》2024年第10期5126-5140,共15页稀有金属（英文版）

基　　金：financially supported by the National Natural Science Foundation of China(No.12204215);Shandong Provincial Natural Science Foundation,China(Nos.ZR2022ME030 and ZR2021QA026)。

摘　　要：The development of stable and highly efficien multifunctional electrocatalysts for the hydrogen evolution reaction(HER),oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are essential for the efficient conversion and storage of renewable energy.The significant advantages of single-atom catalysts,such as strong metal slab interactions,unsaturated coordination and efficient atomic utilization,have opened new avenues for designing multifunctional catalysts.Herein,based on density functional theory,a single atom doped PdPX system was designed as a multifunctional electrocatalyst,which demonstrated the synergistic effect between defects and transition metal atoms and led to enhanced catalytic performance.The results showed that PdPS/PdPSe with P/X vacancy,PdPTe with P/Pd vacancy and Co/Rh/Ir@PdPX exhibited promising HER activity.Co@PdPS(Se),with an overpotential of 0.56(0.44)V,was predicted to be a promising OER catalyst.Moreover,Rh(Ir)@PdPS(Se)catalysts exhibited efficient catalytic properties for ORR Besides,Co@PdPS(Se),Rh(Ir)@PdPS~(V(S)),Co@PdP-Se~(V(Se))and Ir@PdPS~(V(S)-1)exihibited multifunctional catalytic performance with moderate overpotential.Next,the origin of catalytic activity was revealed by using the crystal orbital Hamilton populations theory.For a strong adsorption system,proper filling of the anti-bonding state can increase the energy of the system,weaken the adsorption strength,and facilitate the desorption of intermediates Conversely,augmenting bonding states can enhance its adsorption capacity.These findings provide theoretica guidance for the design and fabrication of novel multifunctional electrocatalysts in terms of filling of bondingstate.

关 键 词：ELECTROCATALYST Two-dimensional PdPX Water splitting Density functional theory 

分 类 号：TQ426[化学工程]