In order to realize electrochemical upgrading and improve the energy conversion efficiency,an ingenious strategy of constructing a thermodynamically favorable oxidation reaction to replace oxygen evolution reaction(OE...In order to realize electrochemical upgrading and improve the energy conversion efficiency,an ingenious strategy of constructing a thermodynamically favorable oxidation reaction to replace oxygen evolution reaction(OER)is proposed.展开更多
Revealing the structure-performance relationships of the molecularly dispersed heterogenized metallomacrocycles(MDHMs)withπ-conjugated heterojunctions is of great,yet largely unmet,significance for realizing the rati...Revealing the structure-performance relationships of the molecularly dispersed heterogenized metallomacrocycles(MDHMs)withπ-conjugated heterojunctions is of great,yet largely unmet,significance for realizing the rational regulation of selectivity,Faradaic efficiency,and durability in the electrochemical CO_(2) reduction reaction(CO_(2)RR).Herein,we describe new insights into the molecularstructure sensitivity of the electrochemical CO_(2)RR over the MDHMs through peripherally functionalizing the heterogenized nickel phthalocyanines with diverse methylimidazole groups.As studied experimentally and theoretically,the heterointerfacial effect and self-built microenvironment of the MDHMs are significantly modulated by accurate structural clipping at the molecular level,predominately steering their electrocatalytic performance for CO_(2)-to-CO conversion in both H-type and flow electrolytic cells.Particularly,the optimized MDHM,2MIMCβNiPc/CNT,displays a significantly improved electrocatalytic performance for CO_(2)RR with near-unity Faradaic efficiency and large current density.Furthermore,the paired electrolysis systems with the MDHMs as the multifunctional electrocatalysts was developed for making full use of the anodic and cathodic reactions,which shows a new and profitable prospect for energy optimization,pollutant regeneration,and green electrosynthesis in a modular form,and also provides guidance for the design and synthesis of novel effi-cient yet economical electrocatalysts.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.21901246 and 22175174)the Natural Science Foundation of Fujian Province(Nos.2020J01116 and 2021J06033)。
文摘In order to realize electrochemical upgrading and improve the energy conversion efficiency,an ingenious strategy of constructing a thermodynamically favorable oxidation reaction to replace oxygen evolution reaction(OER)is proposed.
基金grateful for the financial support of the National Key R&D Program of China(grant no.2021YFA1500402)the National Natural Science Foundation of China(grant nos.21901246,22105203,and 22175174)the Natural Science Foundation of Fujian Province(grant nos.2020J01116 and 2021J06033).
文摘Revealing the structure-performance relationships of the molecularly dispersed heterogenized metallomacrocycles(MDHMs)withπ-conjugated heterojunctions is of great,yet largely unmet,significance for realizing the rational regulation of selectivity,Faradaic efficiency,and durability in the electrochemical CO_(2) reduction reaction(CO_(2)RR).Herein,we describe new insights into the molecularstructure sensitivity of the electrochemical CO_(2)RR over the MDHMs through peripherally functionalizing the heterogenized nickel phthalocyanines with diverse methylimidazole groups.As studied experimentally and theoretically,the heterointerfacial effect and self-built microenvironment of the MDHMs are significantly modulated by accurate structural clipping at the molecular level,predominately steering their electrocatalytic performance for CO_(2)-to-CO conversion in both H-type and flow electrolytic cells.Particularly,the optimized MDHM,2MIMCβNiPc/CNT,displays a significantly improved electrocatalytic performance for CO_(2)RR with near-unity Faradaic efficiency and large current density.Furthermore,the paired electrolysis systems with the MDHMs as the multifunctional electrocatalysts was developed for making full use of the anodic and cathodic reactions,which shows a new and profitable prospect for energy optimization,pollutant regeneration,and green electrosynthesis in a modular form,and also provides guidance for the design and synthesis of novel effi-cient yet economical electrocatalysts.
