The continuous depletion of fossil fuels and the effects of climate change have encouraged prompt action to attain carbon neutrality.Technologies that transform and store renewable energy are crucial for creating a su...The continuous depletion of fossil fuels and the effects of climate change have encouraged prompt action to attain carbon neutrality.Technologies that transform and store renewable energy are crucial for creating a sustainable society,which is independent of fossil fuels.In this regard,electrochemical water splitting based on the oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is an attractive technique for producing carbon-free hydrogen fuels.Additionally,rechargeable metal–air batteries(MABs)are another intriguing way for renewable energy storage through reversible oxygen reactions(OER and the oxygen reduction reaction,ORR).Herein,we comprehensively review bifunctional electrocatalysts for water splitting(HER and OER)and MABs(OER and ORR),particularly 2D carbon material-derived heterostructures.The synthesis and properties of 2D carbon materials and their energy conversion and storage mechanisms are discussed to highlight the bifunc-tionality of the heterostructures.Recent studies on bifunctional electrocatalysts based on 2D carbon-derived heterostructures are also reviewed.Finally,perspectives for future studies and multifunctional catalysts are presented.展开更多
Herein,we have designed a highly active and robust trifunctional electrocatalyst derived from Prussian blue analogs,where Co_(4)N nanoparticles are encapsulated by Fe embedded in N-doped carbon nanocubes to synthesize...Herein,we have designed a highly active and robust trifunctional electrocatalyst derived from Prussian blue analogs,where Co_(4)N nanoparticles are encapsulated by Fe embedded in N-doped carbon nanocubes to synthesize hierarchically structured Co_(4)N@Fe/N-C for rechargeable zinc-air batteries and overall water-splitting electrolyzers.As confirmed by theoretical and experimental results,the high intrinsic oxygen reduction reaction,oxygen evolution reaction,and hydrogen evolution reaction activities of Co_(4)N@Fe/N-C were attributed to the formation of the heterointerface and the modulated local electronic structure.Moreover,Co_(4)N@Fe/N-C induced improvement in these trifunctional electrocatalytic activities owing to the hierarchical hollow nanocube structure,uniform distribution of Co_(4)N,and conductive encapsulation by Fe/N-C.Thus,the rechargeable zinc-air battery with Co_(4)N@Fe/N-C delivers a high specific capacity of 789.9 mAh g^(-1) and stable voltage profiles over 500 cycles.Furthermore,the overall water electrolyzer with Co_(4)N@Fe/N-C achieved better durability and rate performance than that with the Pt/C and IrO2 catalysts,delivering a high Faradaic efficiency of 96.4%.Along with the great potential of the integrated water electrolyzer powered by a zinc-air battery for practical applications,therefore,the mechanistic understanding and active site identification provide valuable insights into the rational design of advanced multifunctional electrocatalysts for energy storage and conversion.展开更多
Herein,we report the molecular engineering of anion-fluxing polymeric metal phthalocyanines(MTPs)by controlling the types of metal centers and incorporating lithiophilic linkers to achieve ultrastable Li metal batteri...Herein,we report the molecular engineering of anion-fluxing polymeric metal phthalocyanines(MTPs)by controlling the types of metal centers and incorporating lithiophilic linkers to achieve ultrastable Li metal batteries.Spectroscopic characterization,cryogenic transmission electron microscopy,and computational simulations demonstrate that the Co-N_(4) sites of Co in the incorporated MTP(CoTP)facilitate the local accumulation and directional flux of TFSI anions,inducing the formation of uniform,dense LiF-rich solid electrolyte interphases.As a result of this interfacial chemistry,symmetric cells with CoTP@CC-Li exhibited outstanding cycling stability,exceeding 2500 h at 1 mA cm^(-2) and 1 mAh cm^(-2).CoTP@CC-Li||LiFePO_(4) full cells operated stably for over 600 cycles under fast charge/discharge conditions,with a high-mass-loading cathode of 20 mg cm^(-2).CoTP@CC-Li||LiFePO_(4) pouch cells demonstrated stable cyclability under demanding practical conditions,including a low N/P ratio of 2.5,high cathode mass loading(23.53 mg cm^(-2)),and lean electrolyte usage(5 g Ah^(-1)).Furthermore,CoTP@CC-enabled anode-free full cells achieved exceptional stability over 500 cycles,even under stringent conditions(NCM811 mass loading of 20 mg cm^(-2) and lean electrolyte usage of 3 g Ah^(-1)).These results highlight the effectiveness of the anion-flux interfacial engineering strategy for enabling stable and reversible Li deposition under demanding conditions.展开更多
基金supported by National R&D Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(Nos.2022R1F1A1072420 and NRF-2020R1A3B2079803).
文摘The continuous depletion of fossil fuels and the effects of climate change have encouraged prompt action to attain carbon neutrality.Technologies that transform and store renewable energy are crucial for creating a sustainable society,which is independent of fossil fuels.In this regard,electrochemical water splitting based on the oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)is an attractive technique for producing carbon-free hydrogen fuels.Additionally,rechargeable metal–air batteries(MABs)are another intriguing way for renewable energy storage through reversible oxygen reactions(OER and the oxygen reduction reaction,ORR).Herein,we comprehensively review bifunctional electrocatalysts for water splitting(HER and OER)and MABs(OER and ORR),particularly 2D carbon material-derived heterostructures.The synthesis and properties of 2D carbon materials and their energy conversion and storage mechanisms are discussed to highlight the bifunc-tionality of the heterostructures.Recent studies on bifunctional electrocatalysts based on 2D carbon-derived heterostructures are also reviewed.Finally,perspectives for future studies and multifunctional catalysts are presented.
基金National Research Foundation of Korea,Grant/Award Numbers:NRF-2020R1A3B2079803,2021R1A2C2007804。
文摘Herein,we have designed a highly active and robust trifunctional electrocatalyst derived from Prussian blue analogs,where Co_(4)N nanoparticles are encapsulated by Fe embedded in N-doped carbon nanocubes to synthesize hierarchically structured Co_(4)N@Fe/N-C for rechargeable zinc-air batteries and overall water-splitting electrolyzers.As confirmed by theoretical and experimental results,the high intrinsic oxygen reduction reaction,oxygen evolution reaction,and hydrogen evolution reaction activities of Co_(4)N@Fe/N-C were attributed to the formation of the heterointerface and the modulated local electronic structure.Moreover,Co_(4)N@Fe/N-C induced improvement in these trifunctional electrocatalytic activities owing to the hierarchical hollow nanocube structure,uniform distribution of Co_(4)N,and conductive encapsulation by Fe/N-C.Thus,the rechargeable zinc-air battery with Co_(4)N@Fe/N-C delivers a high specific capacity of 789.9 mAh g^(-1) and stable voltage profiles over 500 cycles.Furthermore,the overall water electrolyzer with Co_(4)N@Fe/N-C achieved better durability and rate performance than that with the Pt/C and IrO2 catalysts,delivering a high Faradaic efficiency of 96.4%.Along with the great potential of the integrated water electrolyzer powered by a zinc-air battery for practical applications,therefore,the mechanistic understanding and active site identification provide valuable insights into the rational design of advanced multifunctional electrocatalysts for energy storage and conversion.
基金supported by the National Research Foundation(NRF)of Korea grant funded by the Korea government(MSIT)(No.RS-2020-NR049409 and No.RS-2023-00217581)the computational time provided by Korea Institute of Science and Technology Information(KISTI)(KSC-2023-CRE-0414).
文摘Herein,we report the molecular engineering of anion-fluxing polymeric metal phthalocyanines(MTPs)by controlling the types of metal centers and incorporating lithiophilic linkers to achieve ultrastable Li metal batteries.Spectroscopic characterization,cryogenic transmission electron microscopy,and computational simulations demonstrate that the Co-N_(4) sites of Co in the incorporated MTP(CoTP)facilitate the local accumulation and directional flux of TFSI anions,inducing the formation of uniform,dense LiF-rich solid electrolyte interphases.As a result of this interfacial chemistry,symmetric cells with CoTP@CC-Li exhibited outstanding cycling stability,exceeding 2500 h at 1 mA cm^(-2) and 1 mAh cm^(-2).CoTP@CC-Li||LiFePO_(4) full cells operated stably for over 600 cycles under fast charge/discharge conditions,with a high-mass-loading cathode of 20 mg cm^(-2).CoTP@CC-Li||LiFePO_(4) pouch cells demonstrated stable cyclability under demanding practical conditions,including a low N/P ratio of 2.5,high cathode mass loading(23.53 mg cm^(-2)),and lean electrolyte usage(5 g Ah^(-1)).Furthermore,CoTP@CC-enabled anode-free full cells achieved exceptional stability over 500 cycles,even under stringent conditions(NCM811 mass loading of 20 mg cm^(-2) and lean electrolyte usage of 3 g Ah^(-1)).These results highlight the effectiveness of the anion-flux interfacial engineering strategy for enabling stable and reversible Li deposition under demanding conditions.
