Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity...Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity due to the weak adsorption ability to O-containing species.Here,the S-doped VN anchored on N,S-doped multi-dimensional carbon(S-VN/Co/NS-MC)was constructed using the solvothermal and in-situ doping methods.Incorporating sulfur atoms into VN species alters the electron spin state of vanadium in the S-VN/Co/NS-MC for regulating the adsorption energy of vanadium sites to oxygen molecules.The introduced sulfur atoms polarize the V 3d_(z)^(2) electrons,shifting spin-down electrons closer to the Fermi level in the S-VN/Co/NS-MC.Consequently,the introduction of sulfur atoms into VN species enhances the adsorption energy of vanadium sites for oxygen molecules.The*OOH dissociation transitions from being unspontaneous on the VN surface to a spontaneous state on the S-doped VN surface.Then,the ORR barrier on the S-VN/Co/NS-MC surface is reduced.The S-VN/Co/NS-MC demonstrates a higher half-wave potential and limiting current density compared to the VN/Co/N-MC.The S-VN/Co/NS-MC-based liquid ZABs display a power density of 195.7 m W cm^(-2),a specific capacity of 815.7 m A h g^(-1),and a cycling stability exceeding 250 h.The S-VN/Co/NS-MC-based flexible ZABs are successfully employed to charge both a smart watch and a mobile phone.This approach holds promise for advancing the commercial utilization of VN-based catalysts in ZABs.展开更多
An environmentally benign,sustainable,and cost-effective supply of H_(2)O_(2)as a rapidly expanding consumption raw material is highly desired for chemical industries,medical treatment,and household disinfection.The e...An environmentally benign,sustainable,and cost-effective supply of H_(2)O_(2)as a rapidly expanding consumption raw material is highly desired for chemical industries,medical treatment,and household disinfection.The electrocatalytic production route via electrochemical oxygen reduction reaction(ORR)offers a sustainable avenue for the onsite production of H_(2)O_(2)from O2 and H2O.The most crucial and innovative part of such technology lies in the availability of suitable electrocatalysts that promote two-electron(2e^(–))ORR.In recent years,tremendous progress has been achieved in designing efficient,robust,and cost-effective catalyst materials,including noble metals and their alloys,metalfree carbon-based materials,single-atom catalysts,and molecular catalysts.Meanwhile,innovative cell designs have significantly advanced electrochemical applications at the industrial level.This review summarizes fundamental basics and recent advances in H_(2)O_(2)production via 2e^(–)-ORR,including catalyst design,mechanistic explorations,theoretical computations,experimental evaluations,and electrochemical cell designs.Perspectives on addressing remaining challenges are also presented with an emphasis on the large-scale synthesis of H_(2)O_(2)via the electrochemical route.展开更多
The exploration of active and long-lived oxygen reduction reaction(ORR)catalysts for the commercialization of zinc-air batteries are of immense significance but challenging.Herein,the sulfur doped FeWO_(4)embedded in ...The exploration of active and long-lived oxygen reduction reaction(ORR)catalysts for the commercialization of zinc-air batteries are of immense significance but challenging.Herein,the sulfur doped FeWO_(4)embedded in the multi-dimensional nitrogen-doped carbon structure(S-FeWO_(4)/NC)was successfully synthesized.The doped S atoms optimized the charge distribution in FeWO_(4)and enhanced the intrinsic activity.At the same time,S doping accelerated the formation of reaction intermediates during the adsorption reduction of O_(2)on the surface of S-FeWO_(4)/NC.Accordingly,the S-FeWO_(4)/NC catalyst showed more positive half-wave potential(0.85 V)and better stability than that of the FeWO_(4)/NC catalyst.Furthermore,the S-FeWO_(4)/NC-based zinc-air battery exhibited considerable power density of 150.3m W cm^(-2),high specific capacity of 912.7 m A h g^(-1),and prominent cycle stability up to 220 h.This work provides an assistance to the development of cheap and efficient tungsten-based oxygen reduction catalysts and the promotion of its application in the zinc-air battery.展开更多
Due to the poor Fenton reactivity,single-atom Mn-based materials are generally identified as one of the most promising active catalysts for oxygen reduction reaction(ORR).Regulating the electronic density and coordina...Due to the poor Fenton reactivity,single-atom Mn-based materials are generally identified as one of the most promising active catalysts for oxygen reduction reaction(ORR).Regulating the electronic density and coordination environment of atomically dispersed Mn centers is an effective strategy to enhance ORR activity of Mn-based materials.By introducing Zn sites,atomically dispersed Mn centers with multitudes of coordination(including Zn/Mn–Nx and Mn–Nx moieties)can be constructed to form Mn-based ORR catalyst(Zn/Mn-NC)with dual-atom sites.Around Mn–Nx sites,the Zn atoms can effectively modulate the electronic structure and coordination state of Mn centers in Zn/Mn-NC through d–d orbital coupling.The electronic interaction between Zn and Mn sites improves ORR activity,thereby optimizing the oxygen adsorption energy of Mn sites in Zn/Mn-NC and reducing the overall energy barrier.Zn/Mn-NC displays higher ORR half-wave potential than Pt/C(0.89 V vs 0.86 V).The quasi-solid-state zinc-air battery(ZAB)with Zn/Mn-NC as the cathode displayed excellent rechargeability,recyclability,and mechanical robustness.The strategy presented regulates the electronic density and coordination environment of singleatom Mn-based ORR catalysts in quasi-solid-state ZABs.展开更多
With the increasing demand for energy, various emerging energy storage/conversion technologies have gradually penetrated human life, providing numerous conveniences. The practical application efficiency is often affec...With the increasing demand for energy, various emerging energy storage/conversion technologies have gradually penetrated human life, providing numerous conveniences. The practical application efficiency is often affected by the slow kinetics of hydrogen or oxygen electrocatalytic reactions(hydrogen evolution and oxidation reactions, oxygen evolution and reduction reactions) among the emerging devices. Therefore, the researchers devote to finding cost-effective electrocatalysts. Non-noble metal catalysts have low cost and good catalytic activity, but poor stability, agglomeration, dissolution, and other problems will occur after a long cycle, such as transition metal oxides and carbides. Transition metal nitrides(TMNs) stand out among all kinds of non-noble metal catalysts because of the intrinsic platinum-like electrocatalytic activities, relatively high conductivity, and wide range of tunability. In this review, the applications of TMNs in electrocatalytic fields are summarized based on the number of metals contained in TMNs. The practical application potentials of TMNs in fuel cell, water splitting, zinc-air battery and other electrochemical energy storage/conversion devices are also listed. Finally, the design strategies and viewpoints of TMNs-based electrocatalyst are summarized. The potential challenges of TMNs-based electrocatalyst in the development of electrocatalytic energy devices in the future are prospected.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant Nos.22178148,22278193,22075113)the Jiangsu Province and Education Ministry Co-Sponsored Synergistic Innovation Center of Modern Agricultural Equipment(Grant No.XTCX2029)+1 种基金a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutionsthe Postgraduate Research&Practice Innovation Program of Jiangsu Province(Grant No.KYCX22_3691)。
文摘Owing to the distinctive structural characteristics,vanadium nitride(VN)is highly regarded as a catalyst for oxygen reduction reaction(ORR)in zinc-air batteries(ZABs).However,VN exhibits limited intrinsic ORR activity due to the weak adsorption ability to O-containing species.Here,the S-doped VN anchored on N,S-doped multi-dimensional carbon(S-VN/Co/NS-MC)was constructed using the solvothermal and in-situ doping methods.Incorporating sulfur atoms into VN species alters the electron spin state of vanadium in the S-VN/Co/NS-MC for regulating the adsorption energy of vanadium sites to oxygen molecules.The introduced sulfur atoms polarize the V 3d_(z)^(2) electrons,shifting spin-down electrons closer to the Fermi level in the S-VN/Co/NS-MC.Consequently,the introduction of sulfur atoms into VN species enhances the adsorption energy of vanadium sites for oxygen molecules.The*OOH dissociation transitions from being unspontaneous on the VN surface to a spontaneous state on the S-doped VN surface.Then,the ORR barrier on the S-VN/Co/NS-MC surface is reduced.The S-VN/Co/NS-MC demonstrates a higher half-wave potential and limiting current density compared to the VN/Co/N-MC.The S-VN/Co/NS-MC-based liquid ZABs display a power density of 195.7 m W cm^(-2),a specific capacity of 815.7 m A h g^(-1),and a cycling stability exceeding 250 h.The S-VN/Co/NS-MC-based flexible ZABs are successfully employed to charge both a smart watch and a mobile phone.This approach holds promise for advancing the commercial utilization of VN-based catalysts in ZABs.
基金supported by an Australian Research Council(ARC)Discovery Project(DP210103266)This research was supported by an AINSE Ltd.Postgraduate Research Award(PGRA).
文摘An environmentally benign,sustainable,and cost-effective supply of H_(2)O_(2)as a rapidly expanding consumption raw material is highly desired for chemical industries,medical treatment,and household disinfection.The electrocatalytic production route via electrochemical oxygen reduction reaction(ORR)offers a sustainable avenue for the onsite production of H_(2)O_(2)from O2 and H2O.The most crucial and innovative part of such technology lies in the availability of suitable electrocatalysts that promote two-electron(2e^(–))ORR.In recent years,tremendous progress has been achieved in designing efficient,robust,and cost-effective catalyst materials,including noble metals and their alloys,metalfree carbon-based materials,single-atom catalysts,and molecular catalysts.Meanwhile,innovative cell designs have significantly advanced electrochemical applications at the industrial level.This review summarizes fundamental basics and recent advances in H_(2)O_(2)production via 2e^(–)-ORR,including catalyst design,mechanistic explorations,theoretical computations,experimental evaluations,and electrochemical cell designs.Perspectives on addressing remaining challenges are also presented with an emphasis on the large-scale synthesis of H_(2)O_(2)via the electrochemical route.
基金the support of the National Natural Science Foundation of China(Nos.22178148,U21A20328)the Natural Science Foundation of Jiangsu Province(No.BK20191430)+2 种基金the Six Talent Peaks Project in Jiangsu Province(No.XNY-009)the Jiangsu Province and Education Ministry CoSponsored Synergistic Innovation Center of Modern Agricultural Equipment(No.XTCX2029)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘The exploration of active and long-lived oxygen reduction reaction(ORR)catalysts for the commercialization of zinc-air batteries are of immense significance but challenging.Herein,the sulfur doped FeWO_(4)embedded in the multi-dimensional nitrogen-doped carbon structure(S-FeWO_(4)/NC)was successfully synthesized.The doped S atoms optimized the charge distribution in FeWO_(4)and enhanced the intrinsic activity.At the same time,S doping accelerated the formation of reaction intermediates during the adsorption reduction of O_(2)on the surface of S-FeWO_(4)/NC.Accordingly,the S-FeWO_(4)/NC catalyst showed more positive half-wave potential(0.85 V)and better stability than that of the FeWO_(4)/NC catalyst.Furthermore,the S-FeWO_(4)/NC-based zinc-air battery exhibited considerable power density of 150.3m W cm^(-2),high specific capacity of 912.7 m A h g^(-1),and prominent cycle stability up to 220 h.This work provides an assistance to the development of cheap and efficient tungsten-based oxygen reduction catalysts and the promotion of its application in the zinc-air battery.
基金support of the National Natural Science Foundation of China(grant nos.22278193 and 22178148)Jiangsu Province and Education Ministry Cosponsored Synergistic Innovation Center of Modern Agricultural Equipment(grant no.XTCX2029)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Due to the poor Fenton reactivity,single-atom Mn-based materials are generally identified as one of the most promising active catalysts for oxygen reduction reaction(ORR).Regulating the electronic density and coordination environment of atomically dispersed Mn centers is an effective strategy to enhance ORR activity of Mn-based materials.By introducing Zn sites,atomically dispersed Mn centers with multitudes of coordination(including Zn/Mn–Nx and Mn–Nx moieties)can be constructed to form Mn-based ORR catalyst(Zn/Mn-NC)with dual-atom sites.Around Mn–Nx sites,the Zn atoms can effectively modulate the electronic structure and coordination state of Mn centers in Zn/Mn-NC through d–d orbital coupling.The electronic interaction between Zn and Mn sites improves ORR activity,thereby optimizing the oxygen adsorption energy of Mn sites in Zn/Mn-NC and reducing the overall energy barrier.Zn/Mn-NC displays higher ORR half-wave potential than Pt/C(0.89 V vs 0.86 V).The quasi-solid-state zinc-air battery(ZAB)with Zn/Mn-NC as the cathode displayed excellent rechargeability,recyclability,and mechanical robustness.The strategy presented regulates the electronic density and coordination environment of singleatom Mn-based ORR catalysts in quasi-solid-state ZABs.
基金supported by the Natural Science Foundation of Jiangsu Province (No. BK20191430)Six Talent Peaks Project in Jiangsu Province (No. XNY-009)+2 种基金High-tech Research Key Laboratory of Zhenjiang (No. SS2018002)Jiangsu Province Key Laboratory of Intelligent Building Energy Efficiency (No. BEE201904)a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘With the increasing demand for energy, various emerging energy storage/conversion technologies have gradually penetrated human life, providing numerous conveniences. The practical application efficiency is often affected by the slow kinetics of hydrogen or oxygen electrocatalytic reactions(hydrogen evolution and oxidation reactions, oxygen evolution and reduction reactions) among the emerging devices. Therefore, the researchers devote to finding cost-effective electrocatalysts. Non-noble metal catalysts have low cost and good catalytic activity, but poor stability, agglomeration, dissolution, and other problems will occur after a long cycle, such as transition metal oxides and carbides. Transition metal nitrides(TMNs) stand out among all kinds of non-noble metal catalysts because of the intrinsic platinum-like electrocatalytic activities, relatively high conductivity, and wide range of tunability. In this review, the applications of TMNs in electrocatalytic fields are summarized based on the number of metals contained in TMNs. The practical application potentials of TMNs in fuel cell, water splitting, zinc-air battery and other electrochemical energy storage/conversion devices are also listed. Finally, the design strategies and viewpoints of TMNs-based electrocatalyst are summarized. The potential challenges of TMNs-based electrocatalyst in the development of electrocatalytic energy devices in the future are prospected.
