Powered by an inexhaustible supply of solar energy,photoelectrochemical(PEC)nitrogen reduction reaction(NRR)provides an ideal solution for the synthesis of green ammonia(NH_(3)).Although great efforts have been made i...Powered by an inexhaustible supply of solar energy,photoelectrochemical(PEC)nitrogen reduction reaction(NRR)provides an ideal solution for the synthesis of green ammonia(NH_(3)).Although great efforts have been made in the past decades,there are still significant challenges in increasing the NH_(3) yields of the PEC-NRR devices.In addition to the issues of low activity and selectivity similar to electrochemical NRR,the progress of PEC-NRR is also impeded by the limited increase in NH_(3) yields as the electrode is enlarged.Here,we propose an editable electrode design strategy that parallels unit photo-electrodes to achieve a linear increase in NH_(3) yields with electrode active area.We demonstrate that the editable electrode design strategy minimizes the electrode charge transfer resistance,allowing more photo-generated carriers to reach the electrode surface and promote the catalytic reaction.We believe that this editable electrode design strategy provides an avenue to achieve sustainable PEC NH_(3) production.展开更多
Ensemble averaging measurements obscure the link between the electrochemical performance and the specific properties of an individual because of the interplay of inhomogeneity and heterogeneity.Nanocollision electroch...Ensemble averaging measurements obscure the link between the electrochemical performance and the specific properties of an individual because of the interplay of inhomogeneity and heterogeneity.Nanocollision electrochemistry has attracted increasing interest because of its extremely high sensitivity,revealing the intrinsic properties of individual entities that are masked in the traditional ensemble measurements.In this perspective review,we summarized the recent developments in nanocollision-based single entity electrochemistry and photoelectrochemistry,the combined nanocollision electrochemistry with the other complementary techniques,as well as accurate data process.In closing,future challenges,opportunities,and destinations related to nanocollison electrochemistry were discussed.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52071231 and 51722103)the Natural Science Foundation of Tianjin city(No.19JCJQJC61900).
文摘Powered by an inexhaustible supply of solar energy,photoelectrochemical(PEC)nitrogen reduction reaction(NRR)provides an ideal solution for the synthesis of green ammonia(NH_(3)).Although great efforts have been made in the past decades,there are still significant challenges in increasing the NH_(3) yields of the PEC-NRR devices.In addition to the issues of low activity and selectivity similar to electrochemical NRR,the progress of PEC-NRR is also impeded by the limited increase in NH_(3) yields as the electrode is enlarged.Here,we propose an editable electrode design strategy that parallels unit photo-electrodes to achieve a linear increase in NH_(3) yields with electrode active area.We demonstrate that the editable electrode design strategy minimizes the electrode charge transfer resistance,allowing more photo-generated carriers to reach the electrode surface and promote the catalytic reaction.We believe that this editable electrode design strategy provides an avenue to achieve sustainable PEC NH_(3) production.
基金supported by the National Natural Science Foundation of China (21775043, 21421004)the Program of Introducing Talents of Discipline to Universities (B16017)+1 种基金Innovation Program of Shanghai Municipal Education Commission (2017-01-07-00-02E00023)the Fundamental Research Funds for the Central Universities (222201718001, 222201717003)
文摘Ensemble averaging measurements obscure the link between the electrochemical performance and the specific properties of an individual because of the interplay of inhomogeneity and heterogeneity.Nanocollision electrochemistry has attracted increasing interest because of its extremely high sensitivity,revealing the intrinsic properties of individual entities that are masked in the traditional ensemble measurements.In this perspective review,we summarized the recent developments in nanocollision-based single entity electrochemistry and photoelectrochemistry,the combined nanocollision electrochemistry with the other complementary techniques,as well as accurate data process.In closing,future challenges,opportunities,and destinations related to nanocollison electrochemistry were discussed.