Water oxidation, as a mandatory reaction of solar fuels conversion systems, requires the use of light absorbers with electronic properties that are well matched with those of the multi-electron catalyst in order to ac...Water oxidation, as a mandatory reaction of solar fuels conversion systems, requires the use of light absorbers with electronic properties that are well matched with those of the multi-electron catalyst in order to achieve high efficiency. Molecular light absorbers offer flexibility in fine tuning of orbital energetics,and metal oxide nanoparticles have emerged as robust oxygen evolving catalysts. Hence, these material choices offer a promising approach for the development of photocatalytic systems for water oxidation.However, efficient charge transfer coupling of molecular light absorbers and metal oxide nanoparticle catalysts has proven a challenge. Recent new approaches toward the efficient coupling of these components based on synthetic design improvements combined with direct spectroscopic observation and kinetic evaluation of charge transfer processes are discussed.展开更多
Humic-like substances(HULIS)are a major component of brown carbon and consequently play a major role in climate change.In this study,70 PM_(2.5) samples were collected from Xi'an in winter 2019 and summer 2020.Neu...Humic-like substances(HULIS)are a major component of brown carbon and consequently play a major role in climate change.In this study,70 PM_(2.5) samples were collected from Xi'an in winter 2019 and summer 2020.Neutral HULIS(HULIS-n),acidic HULIS(HULIS-a),and high-polarity water-soluble organic compounds(HP-WSOC)were analyzed to determine their carbon concentrations and measure their ultraviolet-visible absorption and infrared spectra.Of the three components,HULIS-n had the highest carbon content in both winter(3.29±1.45μg m^(-3))and in summer(1.38±1.10μg m^(-3)).The semi-quantitative results for the functional groups revealed that HP-WSOC was rich in carboxylic acids and had high aromaticity in winter,whereas HULIS-n was rich in carboxylic acids in summer.Moreover,HULJS-a was richer in nitrate esters and saturated aliphatic hydrocarbons in summer than in winter.The results for specific ultraviolet absorbance(SUVA)and E_(250)/E_(365) revealed that HULIS had higher molecular weight and aromaticity in winter than in summer.HULIS-n dominated in the total light absorption of HULIS+HP-WSOC in both winter(73.08%)and summer(48.57%).Overall,the results on the carbon content,optical properties,and functional groups of WSOCs with differing polarity can improve un-derstanding of environmental and climatic effects.展开更多
Storing reclaimed water in lakes is a widely used method of accommodating changes in the consumption of reclaimed water during wastewater reclamation and reuse. Solar light serves as an important function in degrading...Storing reclaimed water in lakes is a widely used method of accommodating changes in the consumption of reclaimed water during wastewater reclamation and reuse. Solar light serves as an important function in degrading pollutants during storage, and its effect on dissolved organic matter（DOM） was investigated in this study. Solar light significantly decreased the UV_（254） absorbance and fluorescence（FLU） intensity of reclaimed water.However, its effect on the dissolved organic carbon（DOC） value of reclaimed water was very limited. The decrease in the UV_（254） absorbance intensity and FLU excitation–emission matrix regional integration volume（FLU volume） of reclaimed water during solar light irradiation was fit with pseudo-first order reaction kinetics. The decrease of UV_（254） absorbance was much slower than that of the FLU volume. Ultraviolet light in solar light had a key role in decreasing the UV_（254） absorbance and FLU intensity during solar light irradiation. The light fluence-based removal kinetic constants of the UV_（254） and FLU intensity were independent of light intensity. The peaks of the UV_（254） absorbance and FLU intensity with an apparent molecular weight（AMW） of 100 Da to 2000 Da decreased after solar irradiation, whereas the DOC value of the major peaks did not significantly change.展开更多
Time resolved laser spectroscopy and GC/MS were used to investigate the primary processes and the side reactions occurring in benzophenone and chlorothioxanthone/amine systems used as photoinitiators of radical polyme...Time resolved laser spectroscopy and GC/MS were used to investigate the primary processes and the side reactions occurring in benzophenone and chlorothioxanthone/amine systems used as photoinitiators of radical polymerization. The discrepancy observed between the experimental data and the expected behaviour is accounted for by detrimental chemical reaction involving the ketone triplet state, the ketyl radical and the amine-derived radical.展开更多
Light absorber is critical to the further applications of thin film solar cells. Here, we report a facile solution-processed method with an annealing temperature below250°C to fabricate Ag8 SnS6(ATS) light absorb...Light absorber is critical to the further applications of thin film solar cells. Here, we report a facile solution-processed method with an annealing temperature below250°C to fabricate Ag8 SnS6(ATS) light absorber for thin film solar cells. After optimization, the ATS-based thin film solar cells exhibited a reproducible power conversion efficiency(PCE) of about 0.25% and an outstanding long-term stability with 90% of the initial PCE retained after a more than 1,000 h degradation test. This research revealed the potential application of ATS as an earth-abundant, low toxic and chemically stable light absorber in thin film solar cells.展开更多
基金supported by the Director,Office of Science,Office of Basic Energy Sciences,Division of Chemical,Geological and Biosciences of the U.S.Department of Energy under Contract No.DE-AC02-05CH11231
文摘Water oxidation, as a mandatory reaction of solar fuels conversion systems, requires the use of light absorbers with electronic properties that are well matched with those of the multi-electron catalyst in order to achieve high efficiency. Molecular light absorbers offer flexibility in fine tuning of orbital energetics,and metal oxide nanoparticles have emerged as robust oxygen evolving catalysts. Hence, these material choices offer a promising approach for the development of photocatalytic systems for water oxidation.However, efficient charge transfer coupling of molecular light absorbers and metal oxide nanoparticle catalysts has proven a challenge. Recent new approaches toward the efficient coupling of these components based on synthetic design improvements combined with direct spectroscopic observation and kinetic evaluation of charge transfer processes are discussed.
基金supported by the Key R&D project of Shaanxi Province(grant No.2022zDLSF06-07)Chinese Academy of Sciences(CAS)“Light of West China”Program(grant No.XAB2021YN06)the State Key Laboratory of Loess and Quaternary Geology,Institute of Earth Environment,CAs(grant No.SKLLQG2103,SKLLQG2110)was also thanked.
文摘Humic-like substances(HULIS)are a major component of brown carbon and consequently play a major role in climate change.In this study,70 PM_(2.5) samples were collected from Xi'an in winter 2019 and summer 2020.Neutral HULIS(HULIS-n),acidic HULIS(HULIS-a),and high-polarity water-soluble organic compounds(HP-WSOC)were analyzed to determine their carbon concentrations and measure their ultraviolet-visible absorption and infrared spectra.Of the three components,HULIS-n had the highest carbon content in both winter(3.29±1.45μg m^(-3))and in summer(1.38±1.10μg m^(-3)).The semi-quantitative results for the functional groups revealed that HP-WSOC was rich in carboxylic acids and had high aromaticity in winter,whereas HULIS-n was rich in carboxylic acids in summer.Moreover,HULJS-a was richer in nitrate esters and saturated aliphatic hydrocarbons in summer than in winter.The results for specific ultraviolet absorbance(SUVA)and E_(250)/E_(365) revealed that HULIS had higher molecular weight and aromaticity in winter than in summer.HULIS-n dominated in the total light absorption of HULIS+HP-WSOC in both winter(73.08%)and summer(48.57%).Overall,the results on the carbon content,optical properties,and functional groups of WSOCs with differing polarity can improve un-derstanding of environmental and climatic effects.
基金funded by the National Science Fund of China (Nos. 51138006, 51290284)the National High-Tech R&D Program (863) of China (No. 2013AA065205)+1 种基金the Key Science and Technology Project of Shenzhen Water AuthorityThe Collaborative Innovation Center for Regional Environmental Quality also supported this research
文摘Storing reclaimed water in lakes is a widely used method of accommodating changes in the consumption of reclaimed water during wastewater reclamation and reuse. Solar light serves as an important function in degrading pollutants during storage, and its effect on dissolved organic matter（DOM） was investigated in this study. Solar light significantly decreased the UV_（254） absorbance and fluorescence（FLU） intensity of reclaimed water.However, its effect on the dissolved organic carbon（DOC） value of reclaimed water was very limited. The decrease in the UV_（254） absorbance intensity and FLU excitation–emission matrix regional integration volume（FLU volume） of reclaimed water during solar light irradiation was fit with pseudo-first order reaction kinetics. The decrease of UV_（254） absorbance was much slower than that of the FLU volume. Ultraviolet light in solar light had a key role in decreasing the UV_（254） absorbance and FLU intensity during solar light irradiation. The light fluence-based removal kinetic constants of the UV_（254） and FLU intensity were independent of light intensity. The peaks of the UV_（254） absorbance and FLU intensity with an apparent molecular weight（AMW） of 100 Da to 2000 Da decreased after solar irradiation, whereas the DOC value of the major peaks did not significantly change.
文摘Time resolved laser spectroscopy and GC/MS were used to investigate the primary processes and the side reactions occurring in benzophenone and chlorothioxanthone/amine systems used as photoinitiators of radical polymerization. The discrepancy observed between the experimental data and the expected behaviour is accounted for by detrimental chemical reaction involving the ketone triplet state, the ketyl radical and the amine-derived radical.
基金financially supported by the National High Technology Research and Development Program of China(2015AA050602)the Project of Science and Technology Service(STS)Network Initiative,Chinese Academy of Sciences(KFJ-SW-STS-152)
文摘Light absorber is critical to the further applications of thin film solar cells. Here, we report a facile solution-processed method with an annealing temperature below250°C to fabricate Ag8 SnS6(ATS) light absorber for thin film solar cells. After optimization, the ATS-based thin film solar cells exhibited a reproducible power conversion efficiency(PCE) of about 0.25% and an outstanding long-term stability with 90% of the initial PCE retained after a more than 1,000 h degradation test. This research revealed the potential application of ATS as an earth-abundant, low toxic and chemically stable light absorber in thin film solar cells.
