Artificial photosynthetic solar fuels and foodstuffs are an effective and attractive approach for sustaining our society in a green and low‐carbon manner.Although it is a big challenge to develop science and technolo...Artificial photosynthetic solar fuels and foodstuffs are an effective and attractive approach for sustaining our society in a green and low‐carbon manner.Although it is a big challenge to develop science and technology of solar energy conversion,solar fuels including green hydrogen and liquid sunshine such as methanol produced via artificial photosynthesis are an important pathway to reduce the dependence on fossil fuels and the emission of carbon dioxide[1].Artificial photosynthetic systems aim to the efficient conversion of solar energy with water and carbon dioxide into the stable,energy‐dense carriers for chemical industrial supply chains.Furthermore,the advanced foodstuffs,such as biological macromolecules including starch and protein via artificial photosynthesis,will play an important role in animal feed and food industrial feedstock in the future.Therefore,artificial photosynthetic technologies for carbon dioxide conversion and utilization have shed light on the roadmap to move forward to carbon neutrality.展开更多
Ammonia synthesis via the Haber-Bosch process, which has been heralded as the most important invention of the 20 th century, consumes massive amounts of energy, around 1%–2% of the world’s annual energy...Ammonia synthesis via the Haber-Bosch process, which has been heralded as the most important invention of the 20 th century, consumes massive amounts of energy, around 1%–2% of the world’s annual energy consumption. Developing green and sustainable strategies for NH3 synthesis under ambient conditions, using renewable energy, is strongly desired, by both industrial and sci-entific researchers. Artificial photosynthesis for ammonia synthesis, which has recently attracted significant attention, directly produces NH3 from sunlight, and N2 and H2O via photocatalysis. This has been regarded as an ideal, energy-saving and environmentally-benign process for NH3 produc-tion because it can be performed under normal temperature and atmospheric pressure using re-newable solar energy. Although sustainable developments have been achieved since the pioneering work in 1977, many challenging issues（e.g., adsorption and activation of nitrogen molecules on the surface of photocatalysts under mild conditions） have still not been well solved and the photocata-lytic activities are generally low. In this miniature review, I summarize the most recent progress of photocatalytic N2 fixation for ammonia synthesis, focusing specifically on two attractive aspects for adsorption and activation of nitrogen molecules： one is engineering of oxygen vacancies, and the other is mimicking natural nitrogenase for constructing artificial systems for N2 fixation. Several representative works focusing on these aspects in artificial systems have been reported recently, and it has been demonstrated that both factors play more significant roles in photocatalytic N2 re-duction and fixation under ambient conditions. At the end of the review, I also give some remarks and perspective on the existing challenges and future directions in this field.展开更多
The conversion of CO2 and water to value-added chemicals under sunlight irradiation, especially by photoelectrocatalytic reduction process, is always a dream for human beings. A new artificial photosynthesis system co...The conversion of CO2 and water to value-added chemicals under sunlight irradiation, especially by photoelectrocatalytic reduction process, is always a dream for human beings. A new artificial photosynthesis system composed of a metalloporphyrin-functionalized TiO2 photocathode and BiVO4 photoanode can efficiently transform CO2 and water to methanol, which is accompanied by oxygen release. This photoelectrocatalytic system smoothly produces methanol at a rate of 55.5 μM h^–1 cm^– 2, with 0.6 V being the membrane voltage in plants. The production of hydrogen can also be observed when the voltage is more than 0.75 V, due to photocatalysis. Our results evidently indicate that the molecules of metalloporphyrin attached onto the surface of anatase (TiO2) behave as chlorophyll, NADP, and Calvin cycle in plant cells.展开更多
Pt‐loaded graphitic carbon nitride(g‐C_(3)N_(4))is known to be a good photocatalyst for H_(2) evolution under visible light.In most cases,however,sacrificial electron donors such as triethanolamine are required for ...Pt‐loaded graphitic carbon nitride(g‐C_(3)N_(4))is known to be a good photocatalyst for H_(2) evolution under visible light.In most cases,however,sacrificial electron donors such as triethanolamine are required for the water‐splitting operation,and nonsacrificial H_(2) evolution by g‐C_(3)N_(4) remains a challenge.In this work,we investigated the photocatalytic activities of carbon nitride nanosheet(NS‐C_(3)N_(4)),which was prepared by thermal treatment of urea,for nonsacrificial H_(2) evolution using reversible electron donors under visible light(λ>400 nm).Whereas Pt‐loaded NS‐C_(3)N_(4) did not produce H_(2) from aqueous solutions containing I−,Fe^(2+),or[Fe(CN)_(6)]^(4−),modification of the Pt/NS‐C_(3)N_(4) photocatalyst with CrO_(x) led to observable H_(2) evolution.Transmission electron microscopy observations and energy‐dispersive X‐ray spectroscopic analysis suggested that a Pt‐core/CrO_(x)‐shell structure was formed on the NS‐C_(3)N_(4).The CrO_(x)/Pt/NS‐C_(3)N_(4) served as a H_(2)‐evolution photocatalyst for visible‐light‐driven Z‐scheme overall water splitting,in combination with a modified WO_(3) photocatalyst,in the presence of a[Fe(CN)_(6)]^(3−/4−)redox mediator.展开更多
文摘Artificial photosynthetic solar fuels and foodstuffs are an effective and attractive approach for sustaining our society in a green and low‐carbon manner.Although it is a big challenge to develop science and technology of solar energy conversion,solar fuels including green hydrogen and liquid sunshine such as methanol produced via artificial photosynthesis are an important pathway to reduce the dependence on fossil fuels and the emission of carbon dioxide[1].Artificial photosynthetic systems aim to the efficient conversion of solar energy with water and carbon dioxide into the stable,energy‐dense carriers for chemical industrial supply chains.Furthermore,the advanced foodstuffs,such as biological macromolecules including starch and protein via artificial photosynthesis,will play an important role in animal feed and food industrial feedstock in the future.Therefore,artificial photosynthetic technologies for carbon dioxide conversion and utilization have shed light on the roadmap to move forward to carbon neutrality.
文摘Ammonia synthesis via the Haber-Bosch process, which has been heralded as the most important invention of the 20 th century, consumes massive amounts of energy, around 1%–2% of the world’s annual energy consumption. Developing green and sustainable strategies for NH3 synthesis under ambient conditions, using renewable energy, is strongly desired, by both industrial and sci-entific researchers. Artificial photosynthesis for ammonia synthesis, which has recently attracted significant attention, directly produces NH3 from sunlight, and N2 and H2O via photocatalysis. This has been regarded as an ideal, energy-saving and environmentally-benign process for NH3 produc-tion because it can be performed under normal temperature and atmospheric pressure using re-newable solar energy. Although sustainable developments have been achieved since the pioneering work in 1977, many challenging issues（e.g., adsorption and activation of nitrogen molecules on the surface of photocatalysts under mild conditions） have still not been well solved and the photocata-lytic activities are generally low. In this miniature review, I summarize the most recent progress of photocatalytic N2 fixation for ammonia synthesis, focusing specifically on two attractive aspects for adsorption and activation of nitrogen molecules： one is engineering of oxygen vacancies, and the other is mimicking natural nitrogenase for constructing artificial systems for N2 fixation. Several representative works focusing on these aspects in artificial systems have been reported recently, and it has been demonstrated that both factors play more significant roles in photocatalytic N2 re-duction and fixation under ambient conditions. At the end of the review, I also give some remarks and perspective on the existing challenges and future directions in this field.
基金funded by the Natural Science Foundation of Gansu Province(17JR5RA212)the State Key Laboratory of Coal Conversion(J19-20-913-1)~~
文摘The conversion of CO2 and water to value-added chemicals under sunlight irradiation, especially by photoelectrocatalytic reduction process, is always a dream for human beings. A new artificial photosynthesis system composed of a metalloporphyrin-functionalized TiO2 photocathode and BiVO4 photoanode can efficiently transform CO2 and water to methanol, which is accompanied by oxygen release. This photoelectrocatalytic system smoothly produces methanol at a rate of 55.5 μM h^–1 cm^– 2, with 0.6 V being the membrane voltage in plants. The production of hydrogen can also be observed when the voltage is more than 0.75 V, due to photocatalysis. Our results evidently indicate that the molecules of metalloporphyrin attached onto the surface of anatase (TiO2) behave as chlorophyll, NADP, and Calvin cycle in plant cells.
基金supported by the Grants-in-Aid for Scientific Research on the Innovative Area “Mixed Anion” (Project JP16H06441) by the Japan Society for the Promotion of Science (JSPS), and the Japan Association for Chemical Innovation
文摘Pt‐loaded graphitic carbon nitride(g‐C_(3)N_(4))is known to be a good photocatalyst for H_(2) evolution under visible light.In most cases,however,sacrificial electron donors such as triethanolamine are required for the water‐splitting operation,and nonsacrificial H_(2) evolution by g‐C_(3)N_(4) remains a challenge.In this work,we investigated the photocatalytic activities of carbon nitride nanosheet(NS‐C_(3)N_(4)),which was prepared by thermal treatment of urea,for nonsacrificial H_(2) evolution using reversible electron donors under visible light(λ>400 nm).Whereas Pt‐loaded NS‐C_(3)N_(4) did not produce H_(2) from aqueous solutions containing I−,Fe^(2+),or[Fe(CN)_(6)]^(4−),modification of the Pt/NS‐C_(3)N_(4) photocatalyst with CrO_(x) led to observable H_(2) evolution.Transmission electron microscopy observations and energy‐dispersive X‐ray spectroscopic analysis suggested that a Pt‐core/CrO_(x)‐shell structure was formed on the NS‐C_(3)N_(4).The CrO_(x)/Pt/NS‐C_(3)N_(4) served as a H_(2)‐evolution photocatalyst for visible‐light‐driven Z‐scheme overall water splitting,in combination with a modified WO_(3) photocatalyst,in the presence of a[Fe(CN)_(6)]^(3−/4−)redox mediator.
