Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further de...Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.展开更多
Accumulation of hydrogen during anaerobic processes usually results in low decomposition of volatile organic acids(VFAs). On the other hand, hydrogen is a good electron donor for dye reduction, which would help the ...Accumulation of hydrogen during anaerobic processes usually results in low decomposition of volatile organic acids(VFAs). On the other hand, hydrogen is a good electron donor for dye reduction, which would help the acetogenic conversion in keeping low hydrogen concentration. The main objective of the study was to accelerate VFA composition through using azo dye as electron acceptor. The results indicated that the azo dye serving as an electron acceptor could avoid H2 accumulation and accelerate anaerobic digestion of VFAs. After adding the azo dye, propionate decreased from 2400.0 to 689.5 mg/L and acetate production increased from 180.0 to 519.5 mg/L. It meant that the conversion of propionate into acetate was enhanced. Fluorescence in situ hybridization analysis showed that the abundance of propionate-utilizing acetogens with the presence of azo dye was greater than that in a reference without azo dye. The experiments via using glucose as the substrate further demonstrated that the VFA decomposition and the chemical oxygen demand(COD) removal increased by 319.7 mg/L and 23.3% respectively after adding the azo dye. Therefore, adding moderate azo dye might be a way to recover anaerobic system from deterioration due to the accumulation of H2 or VFAs.展开更多
基金support from the Shenzhen Science and Technology Program(No.KQTD20190929173914967,ZDSYS20220527171401003,and JCYJ20200109110416441).
文摘Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic properties.However,the high surface energy limits their synthesis,thus creating significant challenges for further development.In the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal stability.From this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)SACs.Then,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction mechanisms.This review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable batteries.Some light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.
基金supported by the National Crucial Research Project for Water Pollution Control of China (No. 2012ZX07202006)the National Basic Research Program of China (No. 21177015)the New Century Excellent Talent Program of the Ministry of Education of China (No. NCET-10-028)
文摘Accumulation of hydrogen during anaerobic processes usually results in low decomposition of volatile organic acids(VFAs). On the other hand, hydrogen is a good electron donor for dye reduction, which would help the acetogenic conversion in keeping low hydrogen concentration. The main objective of the study was to accelerate VFA composition through using azo dye as electron acceptor. The results indicated that the azo dye serving as an electron acceptor could avoid H2 accumulation and accelerate anaerobic digestion of VFAs. After adding the azo dye, propionate decreased from 2400.0 to 689.5 mg/L and acetate production increased from 180.0 to 519.5 mg/L. It meant that the conversion of propionate into acetate was enhanced. Fluorescence in situ hybridization analysis showed that the abundance of propionate-utilizing acetogens with the presence of azo dye was greater than that in a reference without azo dye. The experiments via using glucose as the substrate further demonstrated that the VFA decomposition and the chemical oxygen demand(COD) removal increased by 319.7 mg/L and 23.3% respectively after adding the azo dye. Therefore, adding moderate azo dye might be a way to recover anaerobic system from deterioration due to the accumulation of H2 or VFAs.