Electrochemical water splitting to produce hydrogen fuel is a promising renewable energy-conversion technique.Large-scale electrolysis of freshwater may deplete water resources and cause water scarcity worldwide.Thus,...Electrochemical water splitting to produce hydrogen fuel is a promising renewable energy-conversion technique.Large-scale electrolysis of freshwater may deplete water resources and cause water scarcity worldwide.Thus,seawater electrolysis is a potential solution to the future energy and water crisis.In seawater electrolysis,it is critical to develop cost-effective electrocatalysts to split seawater without chloride corrosion.Herein,we present zinc-doped nickel iron(oxy)hydroxide nanocubes passivated by negatively charged polyanions(NFZ-PBA-S)that exhibits outstanding catalytic activity,stability,and selectivity for seawater oxidation.Zn dopants and polyanion-rich passivated surface layers in NFZ-PBA-S could effectively repel chlorine ions and enhance corrosion resistance,enabling its excellent catalytic activity and stability for seawater oxidation.展开更多
Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive r...Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways.Here,for highly enhanced PEC H_(2)O_(2)production,we present a conformal amorphous titanyl phosphate(a-TP)overlayer on nanoparticulate TiO_(2)surfaces,achieved via lysozyme-molded in-situ surface reforming.The a-TP overlayer modulates surface adsorption energies for reaction intermediates,favoring WOR for H_(2)O_(2)production over the competing O_(2)evolution reaction.Our density functional theory calculations reveal that a-TP/TiO_(2)exhibits a substantial energy uphill for the O·*formation pathway,which disfavors O_(2)evolution but promotes H_(2)O_(2)production.Additionally,the a-TP overlayer strengthens the built-in electric field,resulting in favorable kinetics.Consequently,a-TP/TiO_(2)exhibits 3.7-fold higher Faraday efficiency(FE)of 63%at 1.76 V vs.reversible hydrogen electrode(RHE)under 1 sun illumination,compared to bare TiO_(2)(17%),representing the highest FE among TiO_(2)-based WOR H_(2)O_(2)production systems.Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.展开更多
A versatile use of a sulfur self-doped biochar derived from Camellia japonica(camellia)flowers is demonstrated as a multifunctional catalyst for overall water splitting and a supercapacitor.The native sulfur content i...A versatile use of a sulfur self-doped biochar derived from Camellia japonica(camellia)flowers is demonstrated as a multifunctional catalyst for overall water splitting and a supercapacitor.The native sulfur content in the camellia flower facilitates in situ self-doping of sulfur,which highly activates the camellia-driven biochar(SA-Came)as a multifunctional catalyst with the enhanced electron-transfer ability and long-term durability.For water splitting,an SA-Came-based electrode is highly stable and shows reaction activities in both hydrogen and oxygen evolution reactions,with overpotentials of 154 and 362 mV at 10 mA cm^(−2),respectively.For supercapacitors,SA-Came achieves a specific capacitance of 125.42 F g^(−1)at 2 A g^(−1)and high cyclic stability in a three-electrode system in a 1 M KOH electrolyte.It demonstrated a high energy density of 34.54 Wh kg^(−1)at a power density of 1600 W kg^(−1)as a symmetric hybrid supercapacitor device with a wide working potential range of 0-1.6 V.展开更多
基金supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF)funded by the Ministry of Science,ICT and Future Planning (2021R1A2C2091497 and 2022R1A2C2010162)supported by“Regional Innovation Strategy (RIS)”through the National Research Foundation of Korea (NRF)funded by the Ministry of Education (MOE) (2022RIS-005)+1 种基金supported by the Ministry of Trade,Industry,and Energy (20018145)supported by KIST Institutional Program (Project Nos.2V09781)。
文摘Electrochemical water splitting to produce hydrogen fuel is a promising renewable energy-conversion technique.Large-scale electrolysis of freshwater may deplete water resources and cause water scarcity worldwide.Thus,seawater electrolysis is a potential solution to the future energy and water crisis.In seawater electrolysis,it is critical to develop cost-effective electrocatalysts to split seawater without chloride corrosion.Herein,we present zinc-doped nickel iron(oxy)hydroxide nanocubes passivated by negatively charged polyanions(NFZ-PBA-S)that exhibits outstanding catalytic activity,stability,and selectivity for seawater oxidation.Zn dopants and polyanion-rich passivated surface layers in NFZ-PBA-S could effectively repel chlorine ions and enhance corrosion resistance,enabling its excellent catalytic activity and stability for seawater oxidation.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government,Ministry of Science and ICT(MSIT)(NRF-2020M3D1A2102837)the Korea Institute of Energy Technology Evaluation and Planning(KETEP)grant funded by the Korea government(MOTIE)(20214000000500,training program of CCUS for the green growth)。
文摘Photoelectrochemical(PEC)H_(2)O_(2)production through water oxidation reaction(WOR)is a promising strategy,however,designing highly efficient and selective photoanode materials remains challenging due to competitive reaction pathways.Here,for highly enhanced PEC H_(2)O_(2)production,we present a conformal amorphous titanyl phosphate(a-TP)overlayer on nanoparticulate TiO_(2)surfaces,achieved via lysozyme-molded in-situ surface reforming.The a-TP overlayer modulates surface adsorption energies for reaction intermediates,favoring WOR for H_(2)O_(2)production over the competing O_(2)evolution reaction.Our density functional theory calculations reveal that a-TP/TiO_(2)exhibits a substantial energy uphill for the O·*formation pathway,which disfavors O_(2)evolution but promotes H_(2)O_(2)production.Additionally,the a-TP overlayer strengthens the built-in electric field,resulting in favorable kinetics.Consequently,a-TP/TiO_(2)exhibits 3.7-fold higher Faraday efficiency(FE)of 63%at 1.76 V vs.reversible hydrogen electrode(RHE)under 1 sun illumination,compared to bare TiO_(2)(17%),representing the highest FE among TiO_(2)-based WOR H_(2)O_(2)production systems.Employing the a-TP overlayer constitutes a promising strategy for controlling reaction pathways and achieving efficient solar-to-chemical energy conversion.
基金National Research Foundation of Korea,Grant/Award Numbers:2016M3D1A1021141,2020R1A2C2006077,2022R1A2C1012419,2021R1A4A1024129,2021R1A5A1030054Ministry of Trade,Industry and Energy(MOTIE,Korea),Grant/Award Number:20213030040590。
文摘A versatile use of a sulfur self-doped biochar derived from Camellia japonica(camellia)flowers is demonstrated as a multifunctional catalyst for overall water splitting and a supercapacitor.The native sulfur content in the camellia flower facilitates in situ self-doping of sulfur,which highly activates the camellia-driven biochar(SA-Came)as a multifunctional catalyst with the enhanced electron-transfer ability and long-term durability.For water splitting,an SA-Came-based electrode is highly stable and shows reaction activities in both hydrogen and oxygen evolution reactions,with overpotentials of 154 and 362 mV at 10 mA cm^(−2),respectively.For supercapacitors,SA-Came achieves a specific capacitance of 125.42 F g^(−1)at 2 A g^(−1)and high cyclic stability in a three-electrode system in a 1 M KOH electrolyte.It demonstrated a high energy density of 34.54 Wh kg^(−1)at a power density of 1600 W kg^(−1)as a symmetric hybrid supercapacitor device with a wide working potential range of 0-1.6 V.