Hydrogen peroxide(H_(2)O_(2))photoproduction in seawater with metal-free photocatalysts derived from biomass materials is a green,sustainable,and ultra environmentally friendly way.However,most photocatalysts are alwa...Hydrogen peroxide(H_(2)O_(2))photoproduction in seawater with metal-free photocatalysts derived from biomass materials is a green,sustainable,and ultra environmentally friendly way.However,most photocatalysts are always corroded or poisoned in seawater,resulting in a significantly reduced catalytic performance.Here,we report the metal-free photocatalysts(RUT-1 to RUT-5)with in-situ generated carbon dots(CDs)from biomass materials(Rutin)by a simple microwave-assisted pyrolysis method.Under visible light(λ≥420 nm,81.6 mW/cm^(2)),the optimized catalyst of RUT-4 is stable and can achieve a high H_(2)O_(2)yield of 330.36μmol/L in seawater,1.78 times higher than that in normal water.New transient potential scanning(TPS)tests are developed and operated to in-situ study the H_(2)O_(2)photoproduction of RUT-4 under operation condition.RUT-4 has strong oxygen(O_(2))absorption capacity,and the O_(2)reduction rate in seawater is higher than that in water.Metal cations in seawater further promote the photo-charge separation and facilitate the photo-reduction reaction.For RUT-4,the conduction band level under operating conditions only satisfies the requirement of O_(2)reduction but not for hydrogen(H2)evolution.This work provides new insights for the in-situ study of photocatalyst under operation condition,and gives a green and sustainable path for the H_(2)O_(2)photoproduction with metal-free catalysts in seawater.展开更多
Oxygen evolution reaction(OER)plays a crucial role in developing energy conversion and adjusting electronic structure of the electrocatalysts can effectively improve the catalytic activity and stability.However,it is ...Oxygen evolution reaction(OER)plays a crucial role in developing energy conversion and adjusting electronic structure of the electrocatalysts can effectively improve the catalytic activity and stability.However,it is a challenge to adjust the electronic structure on two-dimensional iridium dioxide nanosheets(IrO_(2)NS),which have the advantages of high atom utilization.Here,we regulate the surface properties of IrO_(2)NS through sulfonated carbon dots(SCDs)to promote the OER catalytic process.The catalyst IrO_(2)NS/SCDs-2 exhibited excellent catalytic activity with a lower overpotential of 180 mV than IrO_(2)NS(230 mV)at the current density of 10 mA·cm^(-2)in a 0.5 M H2SO4 solution.And after 160 h of stability testing,the overpotential of IrO_(2)NS/SCDs-2 only decreased by 4 mV.Moreover,transient potential scanning test can visually demonstrate that the addition of SCDs improves the conductivity of the catalyst and increases the electron transfer rate.展开更多
基金supported by Natural Science Foundation of Jiangsu Province(No.BK20220028)the National Key Research and Development Program of China(Nos.2020YFA0406104 and 2020YFA0406101)+4 种基金the National Natural Science Foundation of China(Nos.52272043,52271223,52202107,and 52201269)Natural Science Foundation of Jiangsu Province(Nos.BK20210735 and 21KJB430043)the Science and Technology Development Fund,Macao SAR(No.0009/2022/ITP)Shenzhen Science and Technology Plan Project(Collaborative Innovation Special Project,SGDX20220530111203019)Collaborative Innovation Center of Suzhou Nano Science and Technology,the 111 Project,and Suzhou Key Laboratory of Functional Nano and Soft Materials.
文摘Hydrogen peroxide(H_(2)O_(2))photoproduction in seawater with metal-free photocatalysts derived from biomass materials is a green,sustainable,and ultra environmentally friendly way.However,most photocatalysts are always corroded or poisoned in seawater,resulting in a significantly reduced catalytic performance.Here,we report the metal-free photocatalysts(RUT-1 to RUT-5)with in-situ generated carbon dots(CDs)from biomass materials(Rutin)by a simple microwave-assisted pyrolysis method.Under visible light(λ≥420 nm,81.6 mW/cm^(2)),the optimized catalyst of RUT-4 is stable and can achieve a high H_(2)O_(2)yield of 330.36μmol/L in seawater,1.78 times higher than that in normal water.New transient potential scanning(TPS)tests are developed and operated to in-situ study the H_(2)O_(2)photoproduction of RUT-4 under operation condition.RUT-4 has strong oxygen(O_(2))absorption capacity,and the O_(2)reduction rate in seawater is higher than that in water.Metal cations in seawater further promote the photo-charge separation and facilitate the photo-reduction reaction.For RUT-4,the conduction band level under operating conditions only satisfies the requirement of O_(2)reduction but not for hydrogen(H2)evolution.This work provides new insights for the in-situ study of photocatalyst under operation condition,and gives a green and sustainable path for the H_(2)O_(2)photoproduction with metal-free catalysts in seawater.
基金supported by Natural Science Foundation of Jiangsu Province(No.BK20220028)the National Key R&D Program of China(Nos.2020YFA0406104 and 2020YFA0406101)+2 种基金the National Natural Science Foundation of China(Nos.52271223,52272043,52202107,52201269,22273063 and 52302296)the Science and Technology Development Fund,Macao SAR(No.0009/2022/ITP)Collaborative Innovation Center of Suzhou Nano Science and Technology,the 111 Project and Suzhou Key Laboratory of Functional Nano and Soft Materials.
文摘Oxygen evolution reaction(OER)plays a crucial role in developing energy conversion and adjusting electronic structure of the electrocatalysts can effectively improve the catalytic activity and stability.However,it is a challenge to adjust the electronic structure on two-dimensional iridium dioxide nanosheets(IrO_(2)NS),which have the advantages of high atom utilization.Here,we regulate the surface properties of IrO_(2)NS through sulfonated carbon dots(SCDs)to promote the OER catalytic process.The catalyst IrO_(2)NS/SCDs-2 exhibited excellent catalytic activity with a lower overpotential of 180 mV than IrO_(2)NS(230 mV)at the current density of 10 mA·cm^(-2)in a 0.5 M H2SO4 solution.And after 160 h of stability testing,the overpotential of IrO_(2)NS/SCDs-2 only decreased by 4 mV.Moreover,transient potential scanning test can visually demonstrate that the addition of SCDs improves the conductivity of the catalyst and increases the electron transfer rate.