Nanostructured and nanosized materials are widely applied to tackle the pressing challenges associated with energy conversion. In this conceptual review, rather than highlighting separate examples, we aim to give a ge...Nanostructured and nanosized materials are widely applied to tackle the pressing challenges associated with energy conversion. In this conceptual review, rather than highlighting separate examples, we aim to give a general overview about where and how nanostructure design can be beneficial in the three major research fields(photo)thermal chemical energy conversion, electrochemical energy conversion, and solar energy conversion. It will be shown that in many cases the design of catalytically active nanostructures is the main task and that especially for catalysts nanostructure and activity are inseparably linked to each other. Moreover, electrochemical and photochemical processes are complicated by the overlap of multiple processes that all need to be optimized, including in particular light absorption, charge migration,recombination and trapping events and surface processes. It will also be shown how the development of materials for new challenges can often be based on our knowledge on existing materials for related applications.展开更多
Crystalline TiO_2(P25) and isolated titanate species in a ZSM-5 structure(TS-1) were modified with Au and Ag, respectively, and tested in the gas-phase photocatalytic CO_2 reduction under high purity conditions. The n...Crystalline TiO_2(P25) and isolated titanate species in a ZSM-5 structure(TS-1) were modified with Au and Ag, respectively, and tested in the gas-phase photocatalytic CO_2 reduction under high purity conditions. The noble metal modification was performed by photodeposition. Light absorbance properties of the catalysts are examined with UV–Vis spectroscopy before and after the activity test. In the gas-phase photocatalytic CO_2 reduction, it was observed that the catalysts with Ag nanostructures are more active than those with Au nanostructures. It is thus found that the energetic difference between the band gap energy of the semiconductor and the position of the plasmon is influencing the photocatalytic activity.Potentially, plasmon excitation due to visible light absorption results in plasmon resonance energy, which affects the excitation of the semiconductor positively. Therefore, an overlap between band gap energy of the semiconductor and metal plasmon is needed.展开更多
Engineering of defects in semiconductors provides an effective protocol for improving photocatalytic N_(2) conversion efficiency.This review focuses on the state-of-the-art progress in defect engineering of photocatal...Engineering of defects in semiconductors provides an effective protocol for improving photocatalytic N_(2) conversion efficiency.This review focuses on the state-of-the-art progress in defect engineering of photocatalysts for the N_(2) reduction toward ammonia.The basic principles and mechanisms of thermal catalyzed and photon-induced N_(2) reduction are first concisely recapped,including relevant properties of the N_(2) molecule,reaction pathways,and NH3 quantification methods.Subsequently,defect classification,synthesis strategies,and identification techniques are compendiously summarized.Advances of in situ characterization techniques for monitoring defect state during the N_(2) reduction process are also described.Especially,various surface defect strategies and their critical roles in improving the N_(2) photoreduction performance are highlighted,including surface vacancies(i.e.,anionic vacancies and cationic vacancies),heteroatom doping(i.e.,metal element doping and nonmetal element doping),and atomically defined surface sites.Finally,future opportunities and challenges as well as perspectives on further development of defect-engineered photocatalysts for the nitrogen reduction to ammonia are presented.It is expected that this review can provide a profound guidance for more specialized design of defect-engineered catalysts with high activity and stability for nitrogen photochemical fixation.展开更多
文摘Nanostructured and nanosized materials are widely applied to tackle the pressing challenges associated with energy conversion. In this conceptual review, rather than highlighting separate examples, we aim to give a general overview about where and how nanostructure design can be beneficial in the three major research fields(photo)thermal chemical energy conversion, electrochemical energy conversion, and solar energy conversion. It will be shown that in many cases the design of catalytically active nanostructures is the main task and that especially for catalysts nanostructure and activity are inseparably linked to each other. Moreover, electrochemical and photochemical processes are complicated by the overlap of multiple processes that all need to be optimized, including in particular light absorption, charge migration,recombination and trapping events and surface processes. It will also be shown how the development of materials for new challenges can often be based on our knowledge on existing materials for related applications.
文摘Crystalline TiO_2(P25) and isolated titanate species in a ZSM-5 structure(TS-1) were modified with Au and Ag, respectively, and tested in the gas-phase photocatalytic CO_2 reduction under high purity conditions. The noble metal modification was performed by photodeposition. Light absorbance properties of the catalysts are examined with UV–Vis spectroscopy before and after the activity test. In the gas-phase photocatalytic CO_2 reduction, it was observed that the catalysts with Ag nanostructures are more active than those with Au nanostructures. It is thus found that the energetic difference between the band gap energy of the semiconductor and the position of the plasmon is influencing the photocatalytic activity.Potentially, plasmon excitation due to visible light absorption results in plasmon resonance energy, which affects the excitation of the semiconductor positively. Therefore, an overlap between band gap energy of the semiconductor and metal plasmon is needed.
基金This work was supported by the National Natural Science Foundation of China(No.21972010)Beijing Natural Science Foundation(No.2192039)+1 种基金the Foundation of Key Laboratory of Low-Carbon Conversion Science&Engineering,Shanghai Advanced Research Institute,the Chinese Academy of Sciences(No.KLLCCSE-201901,SARI,CAS)Beijing University of Chemical Technology(XK180301,XK1804-2).
文摘Engineering of defects in semiconductors provides an effective protocol for improving photocatalytic N_(2) conversion efficiency.This review focuses on the state-of-the-art progress in defect engineering of photocatalysts for the N_(2) reduction toward ammonia.The basic principles and mechanisms of thermal catalyzed and photon-induced N_(2) reduction are first concisely recapped,including relevant properties of the N_(2) molecule,reaction pathways,and NH3 quantification methods.Subsequently,defect classification,synthesis strategies,and identification techniques are compendiously summarized.Advances of in situ characterization techniques for monitoring defect state during the N_(2) reduction process are also described.Especially,various surface defect strategies and their critical roles in improving the N_(2) photoreduction performance are highlighted,including surface vacancies(i.e.,anionic vacancies and cationic vacancies),heteroatom doping(i.e.,metal element doping and nonmetal element doping),and atomically defined surface sites.Finally,future opportunities and challenges as well as perspectives on further development of defect-engineered photocatalysts for the nitrogen reduction to ammonia are presented.It is expected that this review can provide a profound guidance for more specialized design of defect-engineered catalysts with high activity and stability for nitrogen photochemical fixation.