Metal-organic layers(MOLs), a type of new-emerging two-dimensional ultrathin metal-organic framework materials with large surface areas and highly exposed active sites, have shown promising applications in photocataly...Metal-organic layers(MOLs), a type of new-emerging two-dimensional ultrathin metal-organic framework materials with large surface areas and highly exposed active sites, have shown promising applications in photocatalytic CO_(2) reduction. However, due to a lack of photosensitivity and photooxidation capability, photosensitizers and sacrificial reductants are usually necessary for MOLs-based photocatalytic CO_(2) reduction systems. In this article, by integration of MOLs and quantum dots(QDs), we constructed MOLs-based catalysts with multi-functions of photosensitivity, photoreduction and photooxidation, which thus can serve as photocatalysts for CO_(2) reduction with H_(2)O as an electron donor. Specifically, by an electrostatic self-assembly approach,nickel(Ⅱ)-based MOLs(Ni-MOLs) and CsPbBr_(3)QDs have been assembled, constructing valid Ⅱ-Scheme Ni-MOLs/CsPbBr_(3) heterojunctions with close Ni-MOLs/CsPbBr_(3)heterointerface. Such a close heterointerface shortens the charge transfer distance,thus effectively boosting the charge separation and transfer. As a result, upon illumination by visible light(λ ≥ 400 nm,100 m W cm^(-2)), the optimized photocatalyst shows high efficiency and stability in photochemical CO_(2) reduction in the absence of any photosensitizers and sacrificial reductants. The CO yield reaches as high as 124 μmol g^(-1)in 4 h, over 6 times higher than that achieved by CsPbBr_(3). Additionally, the selectivity reaches 100%. This work provides a new way to construct MOL-based catalysts for artificial photosynthesis.展开更多
基金supported by the National Natural Science Foundation of China (22071182, 22271218, 21931007)the National Key R&D Program of China (2022YFA1502902)。
文摘Metal-organic layers(MOLs), a type of new-emerging two-dimensional ultrathin metal-organic framework materials with large surface areas and highly exposed active sites, have shown promising applications in photocatalytic CO_(2) reduction. However, due to a lack of photosensitivity and photooxidation capability, photosensitizers and sacrificial reductants are usually necessary for MOLs-based photocatalytic CO_(2) reduction systems. In this article, by integration of MOLs and quantum dots(QDs), we constructed MOLs-based catalysts with multi-functions of photosensitivity, photoreduction and photooxidation, which thus can serve as photocatalysts for CO_(2) reduction with H_(2)O as an electron donor. Specifically, by an electrostatic self-assembly approach,nickel(Ⅱ)-based MOLs(Ni-MOLs) and CsPbBr_(3)QDs have been assembled, constructing valid Ⅱ-Scheme Ni-MOLs/CsPbBr_(3) heterojunctions with close Ni-MOLs/CsPbBr_(3)heterointerface. Such a close heterointerface shortens the charge transfer distance,thus effectively boosting the charge separation and transfer. As a result, upon illumination by visible light(λ ≥ 400 nm,100 m W cm^(-2)), the optimized photocatalyst shows high efficiency and stability in photochemical CO_(2) reduction in the absence of any photosensitizers and sacrificial reductants. The CO yield reaches as high as 124 μmol g^(-1)in 4 h, over 6 times higher than that achieved by CsPbBr_(3). Additionally, the selectivity reaches 100%. This work provides a new way to construct MOL-based catalysts for artificial photosynthesis.
