The integration of microorganisms and photosensitizers presents a promising approach to chemical production utilizing solar energy.However,the current system construction process remains complex.Herein,we introduce a ...The integration of microorganisms and photosensitizers presents a promising approach to chemical production utilizing solar energy.However,the current system construction process remains complex.Herein,we introduce a straightforward and efficient solar-to-chemical conversion system that combines the dissolved photosensitizer Eosin Y with the non-photosynthetic bacterium Moorella thermoacetica.Under light radiation,acetate production increased to 5.1μM h^(-1)μM^(-1)catalyst,exceeding the previously reported maximum by 5.9-fold,with a quantum efficiency of 17.6%.The soluble photosensitizer EY can penetrate the cell and directly engage in intracellular energy metabolism,significantly enhancing intracellular ATP and NADPH/NADP^(+)levels.Within this biohybrid system,sacrificial agent triethanolamine played a dual role:(1)providing continuous photoelectron generation by Eosin Y,enhancing intracellular reducing power,and facilitating carbon fixation via the Wood-Ljungdahl pathway;and(2)its oxidation product,formaldehyde,served as a critical intermediate and a direct precursor for methylenetetrahydrofolate in the Wood-Ljungdahl pathway,consequently simplifying reaction steps and markedly boosting acetate yield.This study provides a simple microorganism-photosensitizer biohybrid system to produce acetate and light on the multifaceted roles of sacrificial agents,paving the development of efficient solar energy conversion with nonphotosynthetic bacteria.展开更多
Silica aerogel was prepared by a sol-gel method with combination of freeze drying.The aerogel was filled with TiCl4 in autoclave and used to fabricate a hierarchical structure of TiO_(2) nanofiber shell and SiO_(2) ae...Silica aerogel was prepared by a sol-gel method with combination of freeze drying.The aerogel was filled with TiCl4 in autoclave and used to fabricate a hierarchical structure of TiO_(2) nanofiber shell and SiO_(2) aerogel core(SiO_(2)@TiO_(2)).The TiO_(2) nanofibers with a diameter of 10-15 nm were highly crystalline and mainly grew along the(101)or(001)planes,favoring charge migration along the growth axis of the fibers.The photoluminescence(PL)emission spectra show that the TiO_(2) nanofibers exhibited much lower PL intensity than P25.The free standing TiO2 nanofibers loaded with CuO had a band gap of 3.04 eV.When CuO was hierarchically loaded on the nanofiber surface and into the aerogel core(SiO_(2)/CuO@TiO_(2)/CuO),the absorption edge significantly red shifted,and the band gap was further narrowed to 2.66 eV.Meanwhile,Fe^(3+)implanted TiO_(2) nanofibers on the aerogel surface(SiO_(2)@Fe-TiO_(2))were also fabricated in the same strategy.The CuO loaded nanofibers(SiO_(2)/CuO@Fe-TiO_(2)/CuO)had a band gap of 2.62 eV.The photocatalytic reduction of CO_(2) was performed under light irradiation by a 300 W Xe-lamp for 4 h.The methanol yield over the SiO_(2)/CuO@Fe-TiO_(2)/CuO reached~2,400 μmol·gcat^(-1) in the absence of sacrificial agent.展开更多
The reduction of low-concentration carbon dioxide with water to organic fuels is still a huge challenge. In this study, we successfully designed the partially oxidized cobalt nanoparticles coated by the nitrogendoped ...The reduction of low-concentration carbon dioxide with water to organic fuels is still a huge challenge. In this study, we successfully designed the partially oxidized cobalt nanoparticles coated by the nitrogendoped carbon layer(Co@NC) of 2-8 nm via a facile method and then interspersed with different amount of Pt nanoparticles. The Co@NC decorated with 1 wt% Pt exhibits the best ability for COreduction to CHand a CHproduction rate of 14.4 μmol·g·his achieved. It is worth noting that the system is carried out under low-concentration CO(400 ppm) circumstance without any sacrificial agent, which could be meaningful to the design of catalysts for atmospheric COreduction.展开更多
基金supported by the National Natural Science Foundation of China(22236007,22025603,21802133)the Natural Science Foundation of Xiamen,China(3502Z20227241)。
文摘The integration of microorganisms and photosensitizers presents a promising approach to chemical production utilizing solar energy.However,the current system construction process remains complex.Herein,we introduce a straightforward and efficient solar-to-chemical conversion system that combines the dissolved photosensitizer Eosin Y with the non-photosynthetic bacterium Moorella thermoacetica.Under light radiation,acetate production increased to 5.1μM h^(-1)μM^(-1)catalyst,exceeding the previously reported maximum by 5.9-fold,with a quantum efficiency of 17.6%.The soluble photosensitizer EY can penetrate the cell and directly engage in intracellular energy metabolism,significantly enhancing intracellular ATP and NADPH/NADP^(+)levels.Within this biohybrid system,sacrificial agent triethanolamine played a dual role:(1)providing continuous photoelectron generation by Eosin Y,enhancing intracellular reducing power,and facilitating carbon fixation via the Wood-Ljungdahl pathway;and(2)its oxidation product,formaldehyde,served as a critical intermediate and a direct precursor for methylenetetrahydrofolate in the Wood-Ljungdahl pathway,consequently simplifying reaction steps and markedly boosting acetate yield.This study provides a simple microorganism-photosensitizer biohybrid system to produce acetate and light on the multifaceted roles of sacrificial agents,paving the development of efficient solar energy conversion with nonphotosynthetic bacteria.
基金The authors acknowledgement the financial supports from the Key R&D Planning Project of Hainan Province(No.ZDYF2020015)the Research Lab Construction of Hainan University(No.ZY2019HN09)the National Natural Science Foundation of China(No.51761010).
文摘Silica aerogel was prepared by a sol-gel method with combination of freeze drying.The aerogel was filled with TiCl4 in autoclave and used to fabricate a hierarchical structure of TiO_(2) nanofiber shell and SiO_(2) aerogel core(SiO_(2)@TiO_(2)).The TiO_(2) nanofibers with a diameter of 10-15 nm were highly crystalline and mainly grew along the(101)or(001)planes,favoring charge migration along the growth axis of the fibers.The photoluminescence(PL)emission spectra show that the TiO_(2) nanofibers exhibited much lower PL intensity than P25.The free standing TiO2 nanofibers loaded with CuO had a band gap of 3.04 eV.When CuO was hierarchically loaded on the nanofiber surface and into the aerogel core(SiO_(2)/CuO@TiO_(2)/CuO),the absorption edge significantly red shifted,and the band gap was further narrowed to 2.66 eV.Meanwhile,Fe^(3+)implanted TiO_(2) nanofibers on the aerogel surface(SiO_(2)@Fe-TiO_(2))were also fabricated in the same strategy.The CuO loaded nanofibers(SiO_(2)/CuO@Fe-TiO_(2)/CuO)had a band gap of 2.62 eV.The photocatalytic reduction of CO_(2) was performed under light irradiation by a 300 W Xe-lamp for 4 h.The methanol yield over the SiO_(2)/CuO@Fe-TiO_(2)/CuO reached~2,400 μmol·gcat^(-1) in the absence of sacrificial agent.
基金financially supported by the National Natural Science Foundation of China(Nos.51772312 and 51472260)the Environmental Functional Materials Innovation Team of Ministry of Education(IRT 16R49)the International Joint Laboratory on Resource Chemistry(IJLRC)
文摘The reduction of low-concentration carbon dioxide with water to organic fuels is still a huge challenge. In this study, we successfully designed the partially oxidized cobalt nanoparticles coated by the nitrogendoped carbon layer(Co@NC) of 2-8 nm via a facile method and then interspersed with different amount of Pt nanoparticles. The Co@NC decorated with 1 wt% Pt exhibits the best ability for COreduction to CHand a CHproduction rate of 14.4 μmol·g·his achieved. It is worth noting that the system is carried out under low-concentration CO(400 ppm) circumstance without any sacrificial agent, which could be meaningful to the design of catalysts for atmospheric COreduction.
