The design of cost-effective electrocatalysts is an open challenging for oxygen evolution reaction(OER)due to the“stable-oractive”dilemma.Zirconium dioxide(ZrO_(2)),a versatile and low-cost material that can be stab...The design of cost-effective electrocatalysts is an open challenging for oxygen evolution reaction(OER)due to the“stable-oractive”dilemma.Zirconium dioxide(ZrO_(2)),a versatile and low-cost material that can be stable under OER operating conditions,exhibits inherently poor OER activity from experimental observations.Herein,we doped a series of metal elements to regulate the ZrO_(2)catalytic activity in OER via spin-polarized density functional theory calculations with van der Waals interactions.Microkinetic modeling as a function of the OER activity descriptor(G_(O*)-G_(HO*))displays that 16 metal dopants enable to enhance OER activities over a thermodynamically stable ZrO_(2)surface,among which Fe and Rh(in the form of single-atom dopant)reach the volcano peak(i.e.the optimal activity of OER under the potential of interest),indicating excellent OER performance.Free energy diagram calculations,density of states,and ab initio molecular dynamics simulations further showed that Fe and Rh are the effective dopants for ZrO_(2),leading to low OER overpotential,high conductivity,and good stability.Considering cost-effectiveness,single-atom Fe doped ZrO_(2)emerged as the most promising catalyst for OER.This finding offers a valuable perspective and reference for experimental researchers to design cost-effective catalysts for the industrial-scale OER production.展开更多
The attractive energy density of lithium-sulfur(Li-S)batteries makes them desirable energy storage systems;however,the slow reaction kinetics and formation of lithium dendrites prevent them from reaching full potentia...The attractive energy density of lithium-sulfur(Li-S)batteries makes them desirable energy storage systems;however,the slow reaction kinetics and formation of lithium dendrites prevent them from reaching full potential.To address this issue,hierarchical porous carbon nanofibers network containing Zn single atoms(ZnSA@HPCNF)is synthesized by electrospinning and carbonization.This structure serves as the main anode body,providing excellent chemical anchoring and lipophilicity.The uniform distribution of Zn single atoms and N4coordination supports uniform deposition and continuous plating/stripping of lithium.The results show that the Li|Li/ZnSA@HPCNF symmetrical battery presents stable and low overpotential during 700-and 900-h iterative plating/stripping process at1 and 5 mA·cm^(-2),respectively.Furthermore,the S/CNT||Li/ZnSA@HPCNF full cell shows good flexibility,reversible capacity and cycling stability.This work provides a lithium host strategy based on single-atom dispersed hierarchical porous carbon network,enabling the design of rational lithium metal anodes for use in flexible Li-S full cells.展开更多
基金the funding support from the Research Grants Council of the Hong Kong Special Administrative Region,China[Project No.CityU11308923]the Basic Research Project from Shenzhen Science and Technology Innovation Committee in Shenzhen,China(No.JCYJ20210324134012034)+5 种基金the Applied Research Grant of City University of Hong Kong(project No.of 9667247)Chow Sang Sang Group Research Fund of City University of Hong Kong(project No.9229123)the funding supported by the Seed Collaborative Research Fund Scheme of State Key Laboratory of Marine Pollution which receives regular research funding from Innovation and Technology Commission(ITC)of the Hong Kong SAR Governmentthe JSPS KAKENHI(No.JP23K13703 and JP23KF0102)the high-level science and technology talents project of Lvliang City(No.2022RC07)foundation of Shanxi supercomputing center of China(No.11sxsc202301).
文摘The design of cost-effective electrocatalysts is an open challenging for oxygen evolution reaction(OER)due to the“stable-oractive”dilemma.Zirconium dioxide(ZrO_(2)),a versatile and low-cost material that can be stable under OER operating conditions,exhibits inherently poor OER activity from experimental observations.Herein,we doped a series of metal elements to regulate the ZrO_(2)catalytic activity in OER via spin-polarized density functional theory calculations with van der Waals interactions.Microkinetic modeling as a function of the OER activity descriptor(G_(O*)-G_(HO*))displays that 16 metal dopants enable to enhance OER activities over a thermodynamically stable ZrO_(2)surface,among which Fe and Rh(in the form of single-atom dopant)reach the volcano peak(i.e.the optimal activity of OER under the potential of interest),indicating excellent OER performance.Free energy diagram calculations,density of states,and ab initio molecular dynamics simulations further showed that Fe and Rh are the effective dopants for ZrO_(2),leading to low OER overpotential,high conductivity,and good stability.Considering cost-effectiveness,single-atom Fe doped ZrO_(2)emerged as the most promising catalyst for OER.This finding offers a valuable perspective and reference for experimental researchers to design cost-effective catalysts for the industrial-scale OER production.
基金financially supported by the Natural Science Foundation of Hebei Province of China (Nos.E2020202071,B2021202028 and B2020202052)Hebei Higher Education Teaching Reform Research and Practice Project,China (No.2021GJJG050)+7 种基金State Key Laboratory of Reliability and Intelligence of Electrical Equipment (No.EERI_PI2020007),Hebei University of Technology,Chinathe Outstanding Youth Project of Guangdong Natural Science Foundation (No.2021B1515020051)the Program for the Outstanding Young Talents of Hebei Province,China (Y.Z.)Chunhui Project of Ministry of Education of the People?s Republic of China (No.Z2017010)Department of Science and Technology of Guangdong Province (No.2020B0909030004)Guangdong Innovative and Entrepreneurial Team Program (No.2016ZT06C517)the Science and Technology Program of Guangzhou (No.2019050001)Yunnan Expert Workstation (No.202005AF150028)。
文摘The attractive energy density of lithium-sulfur(Li-S)batteries makes them desirable energy storage systems;however,the slow reaction kinetics and formation of lithium dendrites prevent them from reaching full potential.To address this issue,hierarchical porous carbon nanofibers network containing Zn single atoms(ZnSA@HPCNF)is synthesized by electrospinning and carbonization.This structure serves as the main anode body,providing excellent chemical anchoring and lipophilicity.The uniform distribution of Zn single atoms and N4coordination supports uniform deposition and continuous plating/stripping of lithium.The results show that the Li|Li/ZnSA@HPCNF symmetrical battery presents stable and low overpotential during 700-and 900-h iterative plating/stripping process at1 and 5 mA·cm^(-2),respectively.Furthermore,the S/CNT||Li/ZnSA@HPCNF full cell shows good flexibility,reversible capacity and cycling stability.This work provides a lithium host strategy based on single-atom dispersed hierarchical porous carbon network,enabling the design of rational lithium metal anodes for use in flexible Li-S full cells.
