Unraveling atomic-level active sites of layered photocatalyst towards lowconcentration CO_(2) conversion is still challenging.Herein,the yield and selectivity of photocatalytic CO_(2) reduction of the Aurivillius-rela...Unraveling atomic-level active sites of layered photocatalyst towards lowconcentration CO_(2) conversion is still challenging.Herein,the yield and selectivity of photocatalytic CO_(2) reduction of the Aurivillius-related oxide semiconductor Bi_(2)O_(2)SiO_(3) nanosheet(BOSO)were largely improved using a surface sulfidation strategy.The experiment and theoretical calculation confirmed that surface sulfidation of the Bi_(2)O_(2)SiO_(3) nanosheet(S-BOSO,6.28 nm)redistributed the charge-enriched Bi sites,extended the solar spectrum absorption to the whole visible range,and considerably enhanced the charge separation,in addition to creating new reaction active sites,as compared to pristine BOSO.Subsequently,surface sulfidation played a switchable role,wherein S-BOSO showed a very high CH_(3)OH generation rate(12.78μmol g^(-1) for 4 h,78.6%selectivity)from low-concentration CO_(2)(1000 ppm)under visible light irradiation,which outperforms most of the state-of-the-art photocatalysts under similar conditions.This study presents an atomic-level modification protocol for engineering reactive sites and charge behaviors to promote solar-to-energy conversion.展开更多
基金Natural Science Foundation of Hubei Province,Grant/Award Number:2021CFB242Research Project of Hubei Provincial Department of Education,Grant/Award Number:Q20202501+3 种基金China Postdoctoral Science Foundation,Grant/Award Number:2020M682878National Natural Science Foundation of China,Grant/Award Numbers:51971124,52104254,52171217State Key Laboratory of Electrical Insulation and Power Equipment,Xi'an Jiaotong University,Grant/Award Number:EIPE22208National Postdoctoral Program for Innovative Talents,Grant/Award Number:BX20200222。
文摘Unraveling atomic-level active sites of layered photocatalyst towards lowconcentration CO_(2) conversion is still challenging.Herein,the yield and selectivity of photocatalytic CO_(2) reduction of the Aurivillius-related oxide semiconductor Bi_(2)O_(2)SiO_(3) nanosheet(BOSO)were largely improved using a surface sulfidation strategy.The experiment and theoretical calculation confirmed that surface sulfidation of the Bi_(2)O_(2)SiO_(3) nanosheet(S-BOSO,6.28 nm)redistributed the charge-enriched Bi sites,extended the solar spectrum absorption to the whole visible range,and considerably enhanced the charge separation,in addition to creating new reaction active sites,as compared to pristine BOSO.Subsequently,surface sulfidation played a switchable role,wherein S-BOSO showed a very high CH_(3)OH generation rate(12.78μmol g^(-1) for 4 h,78.6%selectivity)from low-concentration CO_(2)(1000 ppm)under visible light irradiation,which outperforms most of the state-of-the-art photocatalysts under similar conditions.This study presents an atomic-level modification protocol for engineering reactive sites and charge behaviors to promote solar-to-energy conversion.
