Photothermal catalysis represents a promising strategy to utilize the renewable energy source(e.g.,solar energy)to drive chemical reactions more efficiently.Successful and efficient photothermal catalysis relies on th...Photothermal catalysis represents a promising strategy to utilize the renewable energy source(e.g.,solar energy)to drive chemical reactions more efficiently.Successful and efficient photothermal catalysis relies on the availability of ideal photothermal catalysts,which can provide both large areas of catalytically active surface and strong light absorption power simultaneously.Such duplex requirements of a photothermal catalyst exhibit opposing dependence on the size of the catalyst nanoparticles,i.e.,smaller size is beneficial for achieving higher surface area and more active surface,whereas larger size favors the light absorption in the nanoparticles.In this article,we report the synthesis of ultrafine RuOOH nanoparticles with a size of 2–3 nm uniformly dispersed on the surfaces of silica(SiOx)nanospheres of hundreds of nanometers in size to tackle this challenge of forming an ideal photothermal catalyst.The ultrasmall RuOOH nanoparticles exhibit a large surface area as well as the ability to activate adsorbed molecular oxygen.The SiOx nanospheres exhibit strong surface light scattering resonances to enhance the light absorption power of the small RuOOH nanoparticles anchored on the SiOx surface.Therefore,the RuOOH/SiOx composite particles represent a new class of efficient photothermal catalysts with a photothermal energy conversion efficiency of 92.5%for selective aerobic oxidation of benzyl alcohol to benzylaldehyde under ambient conditions.展开更多
Photothermal catalysis utilizing the full solar spectrum to convert CO_(2)and H2O into valuable products holds promise for sustainable energy solutions.However,a major challenge remains in enhancing the photothermal c...Photothermal catalysis utilizing the full solar spectrum to convert CO_(2)and H2O into valuable products holds promise for sustainable energy solutions.However,a major challenge remains in enhancing the photothermal conversion efficiency and carrier mobility of semiconductors like Bi_(2)MoO_(6),which restricts their catalytic performance.Here,we developed a facile strategy to synthesize vertically grown Bi_(2)MoO_(6)(BMO)nanosheets that mimic a bionic butterfly wing scale structure on a biomass-derived carbon framework(BCF).BCF/BMO exhibits high catalytic activity,achieving a CO yield of 165μmol/(g·h),which is an increase of eight times compared to pristine BMO.The wing scale structured BCF/BMO minimizes sunlight reflection and increases the photothermal conversion temperature.BCF consists of crystalline carbon(sp^(2)-C region)dispersed within amorphous carbon(sp^(3)-C hybridized regions),where the crystalline carbon forms“nano-islands”.The N-C-O-Bi covalent bonds at the S-scheme heterojunction interface of BCF/BMO function as electron bridges,connecting the sp^(2)-C nano-islands and enhancing the multilevel built-in electric field and directional trans-interface transport of carriers.As evidenced by DFT calculation,the rich pyridinic-N on the carbon nano-island can establish strong electron coupling with CO_(2),thereby accelerating the cleavage of*COOH and facilitating the formation of CO.Biomass waste-derived carbon nano-islands represent advanced amorphous/crystalline phase materials and offer a simple and low-cost strategy to facilitate carrier migration.This study provides deep insights into carrier migration in photocatalysis and offers guidance for designing efficient heterojunctions inspired by biological systems.展开更多
基金supported by the start-up from Temple University
文摘Photothermal catalysis represents a promising strategy to utilize the renewable energy source(e.g.,solar energy)to drive chemical reactions more efficiently.Successful and efficient photothermal catalysis relies on the availability of ideal photothermal catalysts,which can provide both large areas of catalytically active surface and strong light absorption power simultaneously.Such duplex requirements of a photothermal catalyst exhibit opposing dependence on the size of the catalyst nanoparticles,i.e.,smaller size is beneficial for achieving higher surface area and more active surface,whereas larger size favors the light absorption in the nanoparticles.In this article,we report the synthesis of ultrafine RuOOH nanoparticles with a size of 2–3 nm uniformly dispersed on the surfaces of silica(SiOx)nanospheres of hundreds of nanometers in size to tackle this challenge of forming an ideal photothermal catalyst.The ultrasmall RuOOH nanoparticles exhibit a large surface area as well as the ability to activate adsorbed molecular oxygen.The SiOx nanospheres exhibit strong surface light scattering resonances to enhance the light absorption power of the small RuOOH nanoparticles anchored on the SiOx surface.Therefore,the RuOOH/SiOx composite particles represent a new class of efficient photothermal catalysts with a photothermal energy conversion efficiency of 92.5%for selective aerobic oxidation of benzyl alcohol to benzylaldehyde under ambient conditions.
基金supported by the National Natural Science Foundation of China(52276099,52406219)Graduate Research and Innovation Foundation of Chongqing,China(CYB23034)+2 种基金China Scholarship Council(202406050113)the Australian Research Council(DE230100327)DCCEEW International Clean Innovation Researcher Networks Grant(ICIRN000011)。
文摘Photothermal catalysis utilizing the full solar spectrum to convert CO_(2)and H2O into valuable products holds promise for sustainable energy solutions.However,a major challenge remains in enhancing the photothermal conversion efficiency and carrier mobility of semiconductors like Bi_(2)MoO_(6),which restricts their catalytic performance.Here,we developed a facile strategy to synthesize vertically grown Bi_(2)MoO_(6)(BMO)nanosheets that mimic a bionic butterfly wing scale structure on a biomass-derived carbon framework(BCF).BCF/BMO exhibits high catalytic activity,achieving a CO yield of 165μmol/(g·h),which is an increase of eight times compared to pristine BMO.The wing scale structured BCF/BMO minimizes sunlight reflection and increases the photothermal conversion temperature.BCF consists of crystalline carbon(sp^(2)-C region)dispersed within amorphous carbon(sp^(3)-C hybridized regions),where the crystalline carbon forms“nano-islands”.The N-C-O-Bi covalent bonds at the S-scheme heterojunction interface of BCF/BMO function as electron bridges,connecting the sp^(2)-C nano-islands and enhancing the multilevel built-in electric field and directional trans-interface transport of carriers.As evidenced by DFT calculation,the rich pyridinic-N on the carbon nano-island can establish strong electron coupling with CO_(2),thereby accelerating the cleavage of*COOH and facilitating the formation of CO.Biomass waste-derived carbon nano-islands represent advanced amorphous/crystalline phase materials and offer a simple and low-cost strategy to facilitate carrier migration.This study provides deep insights into carrier migration in photocatalysis and offers guidance for designing efficient heterojunctions inspired by biological systems.
