Photocatalytic anaerobic organic oxidation coupled with H2 evolution represents an advanced solar energy utilization strat-egy for the coproduction of clean fuel and fine chemicals.To achieve a high conversion efficiency,the smart design of efficient catalysts by the right combination of semiconductor light harvesters and co-catalyst is highly required.Herein,we report a composite photocata-lyst composed of noble metal-free transition metal nitride Ni3FeN decorated on 2D ultrathin Znln2S4(ZIS)nanosheets for selective oxi-dation of aromatic alcohols to aldehydes pairing with H2 production.In the composite,ultrathin ZIS serves as a light harvester that greatly shortens the diffusion length of photogenerated charges,while the metallic nitride Ni3FeN acts as an advanced cocatalyst which not only cap-tures the photoelectrons generated from the ultrathin ZIS to promote the charge separation,but also provides active sites to lower the overpo-tential and accelerate the H2 reduction.The best photocatalytic performance is found on ZIS/1.5％M-Ni3FeN,which shows a H2 generation rate of 2427.9 μmol g-1 h-1 and a benzaldehyde(BAD)production rate of 2460 μmol g-1 h-1,about 7.8-fold as high as that of bare ZIS.This work is anticipated to endorse the exploration of transition metal nitrides as high-performance cocatalysts to promote the coupled photocatalytic organic transformation and H2 production.

Mengqing Li;Weiliang Qi;Jiuyang Yu;Lijuan Shen;Xuhui Yang;Siqi Liu;Min-Quan Yang

College of Environmental Science and Engineering,Fujian Key Laboratory of Pollution Control&Resource Reuse,Fujian Normal University,Fuzhou 350007,China;School of Environmental Science and Technology,Dalian University of Technology,Dalian 116024,China

结构化学

[1]Mengqing Li;Weiliang Qi;Jiuyang Yu;Lijuan Shen;Xuhui Yang;Siqi Liu;Min-Quan Yang-.Ultrathin Znln2S4 Nanosheets-Supported Metallic Ni3FeN for Photo-catalytic Coupled Selective Alcohol Oxidation and H2 Evolution)[J].结构化学,2022(12):15-24

Ni3FeN,coproduction,photoelectrons,overpo,endorse

Ultrathin,Znln2S4,Nanosheets,Supported,Metallic,Coupled,Selective,Alcohol,Oxidation,H2,Evolution,Photocatalytic,anaerobic,organic,oxidation,coupled,evolution,represents,advanced,solar,energy,utilization,strat,egy,clean,fuel,fine,chemicals,To,achieve,conversion,efficiency,smart,design,efficient,by,right,combination,semiconductor,light,harvesters,highly,required,Herein,report,composite,composed,noble,free,transition,decorated,2D,ultrathin,ZIS,nanosheets,selective,aromatic,alcohols,aldehydes,pairing,In,serves,as,that,greatly,shortens,diffusion,length,photogenerated,charges,while,metallic,acts,which,not,only,cap,tures,from,promote,separation,but,also,provides,active,sites,lower,tential,accelerate,reduction,best,photocatalytic,performance,found,shows,generation,benzaldehyde,BAD,about,fold,bare,This,work,anticipated,exploration,nitrides,cocatalysts,transformation

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