The selective oxidation of 5-hydroxymethylfurfural(HMF) into 2,5-diformylfuran(DFF) is an important reaction for renewable biomass building blocks. Compared with thermal catalytic processes, photocatalytic production ...The selective oxidation of 5-hydroxymethylfurfural(HMF) into 2,5-diformylfuran(DFF) is an important reaction for renewable biomass building blocks. Compared with thermal catalytic processes, photocatalytic production of DFF from HMF has attracted tremendous attention. Herein, the MoS_(2)/CdIn_(2)S_(4)(MC)flower-like heterojunctions were prepared and considered as photocatalysts for selective oxidation of HMF into DFF under visible-light irradiation in aqueous solution. Results demonstrated MoS_(2) in MC heterojunction could promote the separation of photoexcited electron-hole pairs, while the amount of MoS_(2) dropping was proved influenced on the photocatalytic performance. 80.93% of DFF selectivity was realized when using 12.5% MC as photocatalyst. In addition, the MC catalyst also showed great potential in transformation of other biomass derived benzyl-and furyl-alcohols. The catalytic mechanism suggested that ·O_(2)^(-) was the decisive active radical for HMF oxidation. Therefore, the MC heterojunction could be applied in photocatalytic conversion of biomass to valuable chemicals under ambient condition.展开更多
ZnIn_(2)S_(4) has emerged in water splitting and degradation of dyes due to its good stability and light absorption properties.However,there are still few reports of CO_(2) photoreduction.Herein,we successfully synthe...ZnIn_(2)S_(4) has emerged in water splitting and degradation of dyes due to its good stability and light absorption properties.However,there are still few reports of CO_(2) photoreduction.Herein,we successfully synthesized ZnIn_(2)S_(4) and obtained a series of ZnIn_(2)S_(4)-CdIn_(2)S_(4) heterostructured microspheres through the ion exchange method,and first used them in photocatalytic CO_(2) reduction in noble-metal-free systems.The activity results showed that these ZnIn_(2)S_(4)-CdIn_(2)S_(4) photocatalysts exhibit excellent catalytic activity under visible light,and the best CO yield is as high as 33.57μmol・h^(-1) with a selectivity of 91%.Furthermore,the stability and reusability of ZnIn_(2)S_(4)-CdIn_(2)S_(4) was firmly confirmed by diverse characterizations,including X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),energy-dispersive X-ray spectroscopy(EDX)and N2 adsorption measurements.展开更多
Achieving hydrogen production and simultaneous decomposition of organic pollutants through dual-functional photocatalytic reactions has received increasing attention due to the environmentally friendly and cost-effect...Achieving hydrogen production and simultaneous decomposition of organic pollutants through dual-functional photocatalytic reactions has received increasing attention due to the environmentally friendly and cost-effective characteristics of this approach.In this work,an urchin-like oxygen-doped MoS_(2)/ZnIn_(2)S_(4)(OMS/ZIS)composite was fabricated for the first time using a simple solvothermal method.The unique microstructure with abundant active sites and fast charge transfer channels further shortened the charge migration distance and compressed carrier recombination.The obtained composite exhibited an efficient H2 evolution reaction rate of 12.8 mmol/g/h under visible light,which was nearly times higher than pristine ZnIn_(2)S_(4),and the apparent quantum efficiency was 14.9%(420 nm).The results of the simultaneous photocatalytic H2 evolution and organic pollutant decomposition test were satisfactory,resulting in decomposition efficiencies of resorcinol,tetracycline,and bisphenol A that reached 41.5%,63.5%,and 53.0%after 4 h,respectively,and the highest H2 evolution rate was 672.7 umol/g/h for bisphenol A.Furthermore,natural organic matter(NOM)abundantly found in actual water was adopted as an electron donor for H production under simulated sunlight irradiation,indicating the promising practicability of simultaneous hydrogen evolution and NOM decomposition.Moreover,the mechanisms of the dual-purpose photocatalytic reactions,as well as the synergistic effect between the molecular structures of the organic pollutants and the corresponding adsorption behavior on the photocatalyst surface were illustrated in detail.These obtained results may serve as an inspiration for the rational design of highly efficient,dual-functional photocatalysts in the future.展开更多
基金funded by the National Key Research and Development Program of China ( 2018YFB1501704)the National Natural Science Foundation of China (22078018)the Beijing Natural Science Foundation (2222016)。
文摘The selective oxidation of 5-hydroxymethylfurfural(HMF) into 2,5-diformylfuran(DFF) is an important reaction for renewable biomass building blocks. Compared with thermal catalytic processes, photocatalytic production of DFF from HMF has attracted tremendous attention. Herein, the MoS_(2)/CdIn_(2)S_(4)(MC)flower-like heterojunctions were prepared and considered as photocatalysts for selective oxidation of HMF into DFF under visible-light irradiation in aqueous solution. Results demonstrated MoS_(2) in MC heterojunction could promote the separation of photoexcited electron-hole pairs, while the amount of MoS_(2) dropping was proved influenced on the photocatalytic performance. 80.93% of DFF selectivity was realized when using 12.5% MC as photocatalyst. In addition, the MC catalyst also showed great potential in transformation of other biomass derived benzyl-and furyl-alcohols. The catalytic mechanism suggested that ·O_(2)^(-) was the decisive active radical for HMF oxidation. Therefore, the MC heterojunction could be applied in photocatalytic conversion of biomass to valuable chemicals under ambient condition.
基金supported by the National Key Research and Development Program of China(2021YFA1501500)the National Natural Science Foundation of China(22033008,22220102005,and 22171265)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ103).
文摘催化剂与助催化剂之间的低电荷分离效率严重限制了光催化性能.催化剂与助催化剂之间的强界面相互作用可以提高电荷分离效率.通过引入界面化学键增强组分间的界面相互作用是提高光催化性能的有效手段之一.本文合成了ZnIn_(2)S_(4)(ZIS)/Sv-MoS_(2)光催化剂,ZIS中的S原子与Sv-MoS_(2)中未配位Mo原子之间的键合作用形成了界面Mo–S键,这极大地提高了ZIS的光催化活性.采用不同的NaBH4蚀刻时间制备了MoS_(2-x)h.优化后的Z I S/MoS_(2)-4 h复合材料的产氢速率为7.6 mmol g^(−1)h^(−1),是原ZIS(1.6 mmol g^(−1)h^(−1))的4.75倍,是ZIS/MoS_(2)(3.7 mmol g^(−1)h^(−1))的2.05倍.非凡的光催化活性可归因于光生电子在Mo–S键的作用下更容易从ZIS转移到MoS_(2).光电测量表明,ZIS/MoS_(2)-4h具有有效的电荷转移.本工作揭示了引入界面化学键对ZIS/MoS_(2)光催化活性的影响,为通过界面工程设计优良的助催化剂提供了一种简单有效的方法.
基金This work is supported by National Natural Science Foundation of China(FZUL 21876204 and 22072022)the State Key Laboratory of NBC Protection(SKLNBC2019-14 and SKLNBC2020-18).
文摘ZnIn_(2)S_(4) has emerged in water splitting and degradation of dyes due to its good stability and light absorption properties.However,there are still few reports of CO_(2) photoreduction.Herein,we successfully synthesized ZnIn_(2)S_(4) and obtained a series of ZnIn_(2)S_(4)-CdIn_(2)S_(4) heterostructured microspheres through the ion exchange method,and first used them in photocatalytic CO_(2) reduction in noble-metal-free systems.The activity results showed that these ZnIn_(2)S_(4)-CdIn_(2)S_(4) photocatalysts exhibit excellent catalytic activity under visible light,and the best CO yield is as high as 33.57μmol・h^(-1) with a selectivity of 91%.Furthermore,the stability and reusability of ZnIn_(2)S_(4)-CdIn_(2)S_(4) was firmly confirmed by diverse characterizations,including X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),energy-dispersive X-ray spectroscopy(EDX)and N2 adsorption measurements.
基金supported by the National Key Scientific Instrument and Equipment Development Project of China(No.21627809)the National Natural Science Foundation of China(No.21777056)+2 种基金the Natural Science Foundation of Shandong Province(China)(Nos.ZR2020MB091 and ZR2020MB037)the Youth Innovative Talents Recruitment and Cultivation Program of Shandong Higher Education(China)the Jinan Scientifie Research Leader Workshop Project(China)(No.2018GXRC021).
文摘Achieving hydrogen production and simultaneous decomposition of organic pollutants through dual-functional photocatalytic reactions has received increasing attention due to the environmentally friendly and cost-effective characteristics of this approach.In this work,an urchin-like oxygen-doped MoS_(2)/ZnIn_(2)S_(4)(OMS/ZIS)composite was fabricated for the first time using a simple solvothermal method.The unique microstructure with abundant active sites and fast charge transfer channels further shortened the charge migration distance and compressed carrier recombination.The obtained composite exhibited an efficient H2 evolution reaction rate of 12.8 mmol/g/h under visible light,which was nearly times higher than pristine ZnIn_(2)S_(4),and the apparent quantum efficiency was 14.9%(420 nm).The results of the simultaneous photocatalytic H2 evolution and organic pollutant decomposition test were satisfactory,resulting in decomposition efficiencies of resorcinol,tetracycline,and bisphenol A that reached 41.5%,63.5%,and 53.0%after 4 h,respectively,and the highest H2 evolution rate was 672.7 umol/g/h for bisphenol A.Furthermore,natural organic matter(NOM)abundantly found in actual water was adopted as an electron donor for H production under simulated sunlight irradiation,indicating the promising practicability of simultaneous hydrogen evolution and NOM decomposition.Moreover,the mechanisms of the dual-purpose photocatalytic reactions,as well as the synergistic effect between the molecular structures of the organic pollutants and the corresponding adsorption behavior on the photocatalyst surface were illustrated in detail.These obtained results may serve as an inspiration for the rational design of highly efficient,dual-functional photocatalysts in the future.
