首页|Identification of the highly active Zn-N4 sites with pyrrole/pyridine-N synergistic coordination by dz2+s-band center for electrocatalytic H2O2 production
Identification of the highly active Zn-N4 sites with pyrrole/pyridine-N synergistic coordination by dz2+s-band center for electrocatalytic H2O2 production
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Single metal atoms anchored on nitrogen-doped carbon materials(M-N4)have been identified as effec-tive active sites for catalyzing the two-electron oxygen reduction reaction(2e-ORR).However,the rela-tionship between the local atomic/electronic environments of the M-N4 sites(metal atoms coordinated with different types of N species)and their catalytic activity for 2e-ORR has rarely been elaborated clearly,which imposes significant ambiguity for the rational design of catalysts.Herein,guided by the comprehensive density-functional theory calculations and predictions,a series of Zn-N4 single-atom cat-alysts(SACs)are designed with pyrrole/pyridine-N(NPo/NPd)synergistic coordination and prepared by controlling the pyrolysis temperature(600,700,and 800 ℃).Among them,the dominated Zn-N4 config-urations with rationally combined NPo/NPd coordination show*OOH adsorption strength close to the opti-mal value,much superior to those with mono N species.Thus,the as-prepared catalyst exhibits a high H2O2 selectivity of over 90％both in neutral and alkaline environments,with a superb H2O2 yield of up to 33.63 mol g-1 h-1 in an alkaline with flow cell.More importantly,a new descriptor,dz2+s band center,has been proposed,which is especially feasible for predicting the activity for metal types with fully occu-pied s and d orbitals.This work thus presents clear guidance for the rational design of highly active SACs toward ORR and provides a complement to the d-band theory for more accurately predicting the catalytic activity of the materials.
Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering,Tianjin University,Tianjin 300072,China
Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Science,Shenyang 110016,Liaoning,China
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