The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly...The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly desirable, although it still remains challenging. Herein, we report a facile and reliable route to convert ZIF-8 modified by Fe-phenanthroline into Fe-incorporated and N-doped carbon dodecahedron nanoarchitecture(Fe-NCDNA), in which carbon nanosheets are formed in situ as the building blocks with uniform Fe-N-C species decoration. Systematic electrochemical studies demonstrate that the as-synthesized Fe-NCDNA electrocatalyst possesses highly attractive catalytic features toward the ORR in terms of activity and durability in both alkaline and neutral media. The Zn-air battery with the optimal Fe-NCDNA catalyst as the cathode performs impressively, delivering a power density of 184 m W cm^–2 and a specific capacity of 801 m Ah g^–1;thus, it exhibits great competitive advantages over those of the Zn-air devices employing a Pt-based cathode electrocatalyst.展开更多
Electrosynthesis has recently attracted intensive research attentions and holds great potential in implementing scalable green synthesis thanks to more and more readily accessible renewable electric energy.
Iron single-atom catalysts(Fe SACs)show promise for enhancing zinc-air batteries(ZABs),but their applications are hindered by complex preparation,high cost,and inefficient active site utilization.Here,we present a cos...Iron single-atom catalysts(Fe SACs)show promise for enhancing zinc-air batteries(ZABs),but their applications are hindered by complex preparation,high cost,and inefficient active site utilization.Here,we present a cost-effective,scalable,and environmentally benign approach,using pyrolysis of Ketjen black(KB)with an iron o-phenanthroline complex to create Fe-N-C sites(FeNC-KB).The FeNC-KB catalyst demonstrated high numbers of active sites accessibility and superior oxygen reduction reaction(ORR)properties with a half-wave potential of 0.91 V versus reversible hydrogen electrode(RHE).Notably,its kinetic current density at 0.90 V was 5.1 times that of the 20 wt%Pt/C.In-situ Raman spectroscopy combined with theoretical analysis revealed that the Fe-N_(3)sites exhibited a lower reaction energy barrier,accelerating the formation of*OOH,possessing moderate intermediate adsorption energy,thereby enhancing the ORR activity.When used in a ZAB,the FeNC-KB catalyst achieved an excellent power density of 717mWcm^(-2)and maintained stable operation at 300 mA cm^(-2)for 140 h.These results highlight the efficacy of FeNC-KB catalysts in ZABs and provide a strategy for designing highly active and stable SACs.This advancement has a profound influence on the development of high-performance ZABs and the broader field of energy storage technologies.展开更多
We report a relatively low-temperature molten salt strategy to prepare hollow structured N-doped noble carbon(h-NNC) with highly desirable features of ultra-large surface area(1957 m^2 g^(-1)) and high graphitization,...We report a relatively low-temperature molten salt strategy to prepare hollow structured N-doped noble carbon(h-NNC) with highly desirable features of ultra-large surface area(1957 m^2 g^(-1)) and high graphitization, endowing the h-NNC with high activity toward catalysis of oxygen reduction reaction in acidic medium. The h-NNC is applied as cathode catalyst of an asymmetrical-electrolyte Zn-air battery, which exhibits an open circuit voltage of 2.11 V, a power density up to 270 mW cm^(-2),and an energy density of 1279 W h kg^(-1), behaving advantages over the conventional Zn-air batteries.展开更多
Electrochemical energy devices serve as a vital link in the mutual conversion between chemical energy and electrical energy.This role positions them to be essential for achieving high-efficiency utilization and advanc...Electrochemical energy devices serve as a vital link in the mutual conversion between chemical energy and electrical energy.This role positions them to be essential for achieving high-efficiency utilization and advancement of renewable energy.Electrochemical reactions,including anodic and cathodic reactions,play a crucial role in facilitating the connection between two types of charge carriers:electrons circulating within the external circuit and ions transportation within the internal electrolyte,which ensures the completion of the circuit in electrochemical devices.While electrons are uniform,ions come in various types,we herein propose the concept of hybrid electrochemical energy technologies(h-EETs)characterized by the utilization of different ions as charge carriers of anodic and cathodic reactions.Accordingly,this review aims to explore the fundamentals of emerging hybrid electrochemical energy technologies and recent research advancements.We start with the introduction of the concept and foundational aspects of h-EETs,including the proposed definition,the historical background,operational principles,device configurations,and the underlying principles governing these configurations of the h-EETs.We then discuss how the integration of hybrid charge carriers influences the performance of associated h-EETs,to facilitate an insightful understanding on how ions carriers can be beneficial and effectively implemented into electrochemical energy devices.Furthermore,a special emphasis is placed on offering an overview of the research progress in emerging h-EETs over recent years,including hybrid battery capacitors that extend beyond traditional hybrid supercapacitors,as well as exploration into hybrid fuel cells and hybrid electrolytic synthesis.Finally,we highlight the major challenges and provide anticipatory insights into the future perspectives of developing high-performance h-EETs devices.展开更多
Electrochemical CO_(2)reduction to value-added chemicals or fuels is a prospective strategy for facilitating the closing of the carbon loop.However,there still exist challenges in developing efficient catalysts and op...Electrochemical CO_(2)reduction to value-added chemicals or fuels is a prospective strategy for facilitating the closing of the carbon loop.However,there still exist challenges in developing efficient catalysts and optimizing the electrolyzer components to meet industrial applications.Herein,nitrogen-doped“willow leaf”shaped carbon nanosheets modified with Cu-Ni alloy(CuNi-N-CNS)is designed for electrochemical CO_(2)reduction reaction(CO_(2)RR).展开更多
文摘The application of electrocatalysts for the oxygen reduction reaction(ORR) is vital in a variety of energy conversion technologies. Exploring low-cost ORR catalysts with high activity and long-term stability is highly desirable, although it still remains challenging. Herein, we report a facile and reliable route to convert ZIF-8 modified by Fe-phenanthroline into Fe-incorporated and N-doped carbon dodecahedron nanoarchitecture(Fe-NCDNA), in which carbon nanosheets are formed in situ as the building blocks with uniform Fe-N-C species decoration. Systematic electrochemical studies demonstrate that the as-synthesized Fe-NCDNA electrocatalyst possesses highly attractive catalytic features toward the ORR in terms of activity and durability in both alkaline and neutral media. The Zn-air battery with the optimal Fe-NCDNA catalyst as the cathode performs impressively, delivering a power density of 184 m W cm^–2 and a specific capacity of 801 m Ah g^–1;thus, it exhibits great competitive advantages over those of the Zn-air devices employing a Pt-based cathode electrocatalyst.
基金financially supported by the National Natural Science Foundation of China(Project No.21875253,No.51903235)。
文摘Electrosynthesis has recently attracted intensive research attentions and holds great potential in implementing scalable green synthesis thanks to more and more readily accessible renewable electric energy.
基金supported by the National Natural Science Foundation of China(grant nos.22225902,22109164,and U22A20436)the National Key Research&Development Program of China(grant nos.2022YFE0115900 and 2021YFA1501500).
文摘Iron single-atom catalysts(Fe SACs)show promise for enhancing zinc-air batteries(ZABs),but their applications are hindered by complex preparation,high cost,and inefficient active site utilization.Here,we present a cost-effective,scalable,and environmentally benign approach,using pyrolysis of Ketjen black(KB)with an iron o-phenanthroline complex to create Fe-N-C sites(FeNC-KB).The FeNC-KB catalyst demonstrated high numbers of active sites accessibility and superior oxygen reduction reaction(ORR)properties with a half-wave potential of 0.91 V versus reversible hydrogen electrode(RHE).Notably,its kinetic current density at 0.90 V was 5.1 times that of the 20 wt%Pt/C.In-situ Raman spectroscopy combined with theoretical analysis revealed that the Fe-N_(3)sites exhibited a lower reaction energy barrier,accelerating the formation of*OOH,possessing moderate intermediate adsorption energy,thereby enhancing the ORR activity.When used in a ZAB,the FeNC-KB catalyst achieved an excellent power density of 717mWcm^(-2)and maintained stable operation at 300 mA cm^(-2)for 140 h.These results highlight the efficacy of FeNC-KB catalysts in ZABs and provide a strategy for designing highly active and stable SACs.This advancement has a profound influence on the development of high-performance ZABs and the broader field of energy storage technologies.
基金supported by the 1000 Plan Professorship for Young TalentsHundred Talents Program of Fujian Province+1 种基金the Fujian Science and Technology Key Project (2016H0043)the National Natural Science Foundation of China (21703249, 21701175)
文摘We report a relatively low-temperature molten salt strategy to prepare hollow structured N-doped noble carbon(h-NNC) with highly desirable features of ultra-large surface area(1957 m^2 g^(-1)) and high graphitization, endowing the h-NNC with high activity toward catalysis of oxygen reduction reaction in acidic medium. The h-NNC is applied as cathode catalyst of an asymmetrical-electrolyte Zn-air battery, which exhibits an open circuit voltage of 2.11 V, a power density up to 270 mW cm^(-2),and an energy density of 1279 W h kg^(-1), behaving advantages over the conventional Zn-air batteries.
基金supported by the National Natural Science Foundation of China(22109164,22225902,and U22A20436)the National Key Research&Development Program of China(2022YFE0115900,2021YFA1501500)+2 种基金the CASCommonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(121835KYSB20200039)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021011)Fujian Province Central Government Guides to Science and Technology Development Special Project(2022L3024)。
文摘Electrochemical energy devices serve as a vital link in the mutual conversion between chemical energy and electrical energy.This role positions them to be essential for achieving high-efficiency utilization and advancement of renewable energy.Electrochemical reactions,including anodic and cathodic reactions,play a crucial role in facilitating the connection between two types of charge carriers:electrons circulating within the external circuit and ions transportation within the internal electrolyte,which ensures the completion of the circuit in electrochemical devices.While electrons are uniform,ions come in various types,we herein propose the concept of hybrid electrochemical energy technologies(h-EETs)characterized by the utilization of different ions as charge carriers of anodic and cathodic reactions.Accordingly,this review aims to explore the fundamentals of emerging hybrid electrochemical energy technologies and recent research advancements.We start with the introduction of the concept and foundational aspects of h-EETs,including the proposed definition,the historical background,operational principles,device configurations,and the underlying principles governing these configurations of the h-EETs.We then discuss how the integration of hybrid charge carriers influences the performance of associated h-EETs,to facilitate an insightful understanding on how ions carriers can be beneficial and effectively implemented into electrochemical energy devices.Furthermore,a special emphasis is placed on offering an overview of the research progress in emerging h-EETs over recent years,including hybrid battery capacitors that extend beyond traditional hybrid supercapacitors,as well as exploration into hybrid fuel cells and hybrid electrolytic synthesis.Finally,we highlight the major challenges and provide anticipatory insights into the future perspectives of developing high-performance h-EETs devices.
基金supported by the National key Research&Development Program of China(2022YFE0115900 and 2021YFA1501500)the National Natural Science Foundation of China(No.22225902,U22A20436 and 22209183)+3 种基金the CAS-Commonwealth Scientific and Industrial Research Organization(CSIRO)Joint Research Projects(121835KYSB20200039)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(Grant YLU-DNL Fund 2021011)Fujian Province Central Government Guides to Science and Technology Development Special Project(No.2022L3024)Fujian Natural Science Foundation(2021J01210293).
文摘Electrochemical CO_(2)reduction to value-added chemicals or fuels is a prospective strategy for facilitating the closing of the carbon loop.However,there still exist challenges in developing efficient catalysts and optimizing the electrolyzer components to meet industrial applications.Herein,nitrogen-doped“willow leaf”shaped carbon nanosheets modified with Cu-Ni alloy(CuNi-N-CNS)is designed for electrochemical CO_(2)reduction reaction(CO_(2)RR).
