As a fascinating alternative to the energy-intensive Haber-Bosch process,the electrochemically-driven N_(2) reduction reaction(NRR)utilizing the N_(2) and H_(2)O for the production of NH3 has received enormous attenti...As a fascinating alternative to the energy-intensive Haber-Bosch process,the electrochemically-driven N_(2) reduction reaction(NRR)utilizing the N_(2) and H_(2)O for the production of NH3 has received enormous attention.The development and preparation of promising electrocatalysts are requisite to realize an efficient N_(2) conversion for NH3 production.In this research,we propose a template-assisted strategy to construct the hollow electrocatalyst with controllable morphology.As a paradigm,the hollow Cr_(2)O_(3) nanocatalyst with a uniform size(~170 nm),small cavity and ultrathin shell(~15 nm)is successfully fabricated with this strategy.This promising hollow structure is favourable to trap N_(2) into the cavity,provides abundant active sites to accelerate the three-phase interactions,and facilitates the reactant transfer across the shell.Attributed to these synergetic effects,the designed catalyst displays an outstanding behaviour in N_(2) fixation for NH3 production in ambient condition.In the neutral electrolyte of 0.1 mol·L^(-1) Na_(2)SO_(4),an impressive electrocatalytic performance with the NH3 generation rate of 2.72μg·h^(-1)·cm^(-2) and a high FE of 5.31%is acquired respectively at-0.85 V with the hollow Cr_(2)O_(3) catalyst.Inspired by this work,it is highly expected that this approach could be applied as a universal strategy and extended to fabricating other promising electrocatalysts for realizing highly efficient nitrogen reduction reaction(NRR).展开更多
基金supported by Australian Research Council Discovery Projects(DP170104264 and DP190103548)。
文摘As a fascinating alternative to the energy-intensive Haber-Bosch process,the electrochemically-driven N_(2) reduction reaction(NRR)utilizing the N_(2) and H_(2)O for the production of NH3 has received enormous attention.The development and preparation of promising electrocatalysts are requisite to realize an efficient N_(2) conversion for NH3 production.In this research,we propose a template-assisted strategy to construct the hollow electrocatalyst with controllable morphology.As a paradigm,the hollow Cr_(2)O_(3) nanocatalyst with a uniform size(~170 nm),small cavity and ultrathin shell(~15 nm)is successfully fabricated with this strategy.This promising hollow structure is favourable to trap N_(2) into the cavity,provides abundant active sites to accelerate the three-phase interactions,and facilitates the reactant transfer across the shell.Attributed to these synergetic effects,the designed catalyst displays an outstanding behaviour in N_(2) fixation for NH3 production in ambient condition.In the neutral electrolyte of 0.1 mol·L^(-1) Na_(2)SO_(4),an impressive electrocatalytic performance with the NH3 generation rate of 2.72μg·h^(-1)·cm^(-2) and a high FE of 5.31%is acquired respectively at-0.85 V with the hollow Cr_(2)O_(3) catalyst.Inspired by this work,it is highly expected that this approach could be applied as a universal strategy and extended to fabricating other promising electrocatalysts for realizing highly efficient nitrogen reduction reaction(NRR).