Investigating highly effective electrocatalysts for high-temperature proton exchange membrane fuel cells(HT-PEMFC)requires the resistance to phosphate acid(PA)poisoning at cathodic oxygen reduction reaction(ORR).Recen...Investigating highly effective electrocatalysts for high-temperature proton exchange membrane fuel cells(HT-PEMFC)requires the resistance to phosphate acid(PA)poisoning at cathodic oxygen reduction reaction(ORR).Recent advancements in catalysts have focused on alleviating phosphoric anion adsorption on Pt-based catalysts with modified electronic structure or catalytic interface and developing Fe-N-C based catalysts with immunity of PA poisoning.Fe-N-C-based catalysts have emerged as promising alternatives to Pt-based catalysts,offering significant potential to overcome the characteristic adsorption of phosphate anion on Pt.An overview of these developments provides insights into catalytic mechanisms and facilitates the design of more efficient catalysts.This review begins with an exploration of basic poisoning principles,followed by a critical summary of characterization techniques employed to identified the underlying mechanism of poisoning effect.Attention is then directed to endeavors aimed at enhancing the HT-PEMFC performance by well-designed catalysts.Finally,the opportunities and challenges in developing the anti-PA poisoning strategy and practical HT-PEMFC is discussed.Through these discussions,a comprehensive understanding of PA-poisoning bottlenecks and inspire future research directions is aim to provided.展开更多
The electrocatalytic synthesis of imines through the reductive imination of nitroarenes with aldehydes is a facile,environmentally friendly,and valuable process.In this study,high selectivity electrosynthesis of imine...The electrocatalytic synthesis of imines through the reductive imination of nitroarenes with aldehydes is a facile,environmentally friendly,and valuable process.In this study,high selectivity electrosynthesis of imines was realized through the electrocatalytic C-N coupling reaction between nitroarenes and aryl aldehydes on Co_(9)S_(8)nanoflowers with rich sulfur vacancies(Co_(9)S_(8)-Vs).Comparative experiments revealed that positively charged sulfur vacancies play a pivotal role in boosting catalytic selectivity towards imines.Electron-deficient sulfur vacancies intensified the adsorption of negatively charged Ph-NO_(2),thereby enhancing the conversion rate of the electrochemical nitrobenzene-reduction reaction(eNB-RR).Simultaneously,sulfur vacancies augmented the adsorption capability of negatively charged Ph-CHO,enriching Ph-CHO species at the electrode interface and expediting the Schiff base condensation reaction rate.The experimental results show that the reaction conditions can satisfy the different nitroarenes and aryl aldehydes in the electrocatalytic aqueous-phase system under mild conditions to obtain the corresponding imine products in high selectivity.This study provides a facile and environmentally friendly pathway for future electrocatalytic synthesis of imine.展开更多
文摘Investigating highly effective electrocatalysts for high-temperature proton exchange membrane fuel cells(HT-PEMFC)requires the resistance to phosphate acid(PA)poisoning at cathodic oxygen reduction reaction(ORR).Recent advancements in catalysts have focused on alleviating phosphoric anion adsorption on Pt-based catalysts with modified electronic structure or catalytic interface and developing Fe-N-C based catalysts with immunity of PA poisoning.Fe-N-C-based catalysts have emerged as promising alternatives to Pt-based catalysts,offering significant potential to overcome the characteristic adsorption of phosphate anion on Pt.An overview of these developments provides insights into catalytic mechanisms and facilitates the design of more efficient catalysts.This review begins with an exploration of basic poisoning principles,followed by a critical summary of characterization techniques employed to identified the underlying mechanism of poisoning effect.Attention is then directed to endeavors aimed at enhancing the HT-PEMFC performance by well-designed catalysts.Finally,the opportunities and challenges in developing the anti-PA poisoning strategy and practical HT-PEMFC is discussed.Through these discussions,a comprehensive understanding of PA-poisoning bottlenecks and inspire future research directions is aim to provided.
文摘The electrocatalytic synthesis of imines through the reductive imination of nitroarenes with aldehydes is a facile,environmentally friendly,and valuable process.In this study,high selectivity electrosynthesis of imines was realized through the electrocatalytic C-N coupling reaction between nitroarenes and aryl aldehydes on Co_(9)S_(8)nanoflowers with rich sulfur vacancies(Co_(9)S_(8)-Vs).Comparative experiments revealed that positively charged sulfur vacancies play a pivotal role in boosting catalytic selectivity towards imines.Electron-deficient sulfur vacancies intensified the adsorption of negatively charged Ph-NO_(2),thereby enhancing the conversion rate of the electrochemical nitrobenzene-reduction reaction(eNB-RR).Simultaneously,sulfur vacancies augmented the adsorption capability of negatively charged Ph-CHO,enriching Ph-CHO species at the electrode interface and expediting the Schiff base condensation reaction rate.The experimental results show that the reaction conditions can satisfy the different nitroarenes and aryl aldehydes in the electrocatalytic aqueous-phase system under mild conditions to obtain the corresponding imine products in high selectivity.This study provides a facile and environmentally friendly pathway for future electrocatalytic synthesis of imine.
