Small-scale and decentralized production of H_(2)O_(2)via electrochemical reduction of oxygen is of great benefit,especially for sanitization,air and water purification,as well as for a variety of chemical processes.T...Small-scale and decentralized production of H_(2)O_(2)via electrochemical reduction of oxygen is of great benefit,especially for sanitization,air and water purification,as well as for a variety of chemical processes.The development of low-cost and highperformance catalysts for this reaction remains a key challenge.Carbon-based materials have drawn substantial research efforts in recent years due to their advantageous properties,such as high chemical stability and high tunability in active sites and morphology.Deeper understanding of structure–activity relationships can guide the design of improved catalysts.We hypothesize that mass transport to active sites is of great importance,and herein we use carbon materials with unique flower-like superstructures to achieve high activity and selectivity for O2 reduction to H_(2)O_(2).The abundance of nitrogen active sites controlled by pyrolysis temperature resulted in high catalytic activity and selectivity for oxygen reduction reaction(ORR).The flower superstructure showed higher performance than the spherical nanoparticles due to greater accessibility to the active sites.Chemical activation improves the catalysts’performances further,driving the production of H_(2)O_(2)to a record-setting rate of 816 mmol·gcat^(−1)·h^(−1)using a bulk electrolysis setup.This work demonstrates the development of a highly active catalyst for the sustainable production of H_(2)O_(2)through rational design and synthetic control.The understanding from this work provides further insight into the design of future carbon-based electrocatalysts.展开更多
基金This research was supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,Chemical Sciences,Geosciences,and Biosciences Division,Catalysis Science Program to the SUNCAT Center for Interface Science and Catalysis.Part of this work was performed at the Stanford Nano Shared Facilities,supported by the National Science Foundation under award ECCS-2026822.
文摘Small-scale and decentralized production of H_(2)O_(2)via electrochemical reduction of oxygen is of great benefit,especially for sanitization,air and water purification,as well as for a variety of chemical processes.The development of low-cost and highperformance catalysts for this reaction remains a key challenge.Carbon-based materials have drawn substantial research efforts in recent years due to their advantageous properties,such as high chemical stability and high tunability in active sites and morphology.Deeper understanding of structure–activity relationships can guide the design of improved catalysts.We hypothesize that mass transport to active sites is of great importance,and herein we use carbon materials with unique flower-like superstructures to achieve high activity and selectivity for O2 reduction to H_(2)O_(2).The abundance of nitrogen active sites controlled by pyrolysis temperature resulted in high catalytic activity and selectivity for oxygen reduction reaction(ORR).The flower superstructure showed higher performance than the spherical nanoparticles due to greater accessibility to the active sites.Chemical activation improves the catalysts’performances further,driving the production of H_(2)O_(2)to a record-setting rate of 816 mmol·gcat^(−1)·h^(−1)using a bulk electrolysis setup.This work demonstrates the development of a highly active catalyst for the sustainable production of H_(2)O_(2)through rational design and synthetic control.The understanding from this work provides further insight into the design of future carbon-based electrocatalysts.
