This work describes the use of TiO_(2)nanotubes-based electrodes(TNT)modified with Cu_(2)O nanostructures and gold nanoparticles for the photoelectroreduction of CO_(2)to produce value-added compounds.A thin layer of ...This work describes the use of TiO_(2)nanotubes-based electrodes(TNT)modified with Cu_(2)O nanostructures and gold nanoparticles for the photoelectroreduction of CO_(2)to produce value-added compounds.A thin layer of polydopamine was used as both an adherent agent and an electron transfer mediator,due to itsπ-conjugated electron system.The highest production yield was achieved using a TNT@PDA/Nc/Au40%electrode,with Faradaic efficiencies of 47.4%(110.5μM cm^(-2))and 27.8%(50.4μM cm^(-2))for methanol and methane,respectively.The performance of the photoelectrodes was shown to be Cu_(2)O facet-dependent,with cubic structures leading to greater conversion of CO_(2)to methanol(43%)and methane(27%),compared to the octahedral morphology,while a higher percentage of metallic gold on the nanostructured Cu_(2)O surface was mainly important for CH4production.Density functional theory(DFT)calculations supported these findings,attributing the superior photoelectrocatalytic performance of the TNT@PDA/Nc/Au40%electrode for CH4generation to the formation of an OCH3intermediate bonded to Au atoms.Studies using isotope-labeling and analysis by gas chromatograph-mass(GC-MS)demonstrated that13CO_(2)was the source for photoelectrocatalytic generation of13CH3OH and13CH313CH2OH.展开更多
The photoelectrochemical conversion of CO_(2) into value-added products emerges as an attractive approach to alleviate climate change. One of the main challenges in deploying this technology is, however, the developme...The photoelectrochemical conversion of CO_(2) into value-added products emerges as an attractive approach to alleviate climate change. One of the main challenges in deploying this technology is, however, the development and optimization of(photo)electrodes and photoelectrolyzers. This review focuses on the fabrication processes, structure, and characterization of(photo)electrodes, covering a wide range of fabrication techniques, from rudimentary to automated fabrication processes. The work also highlights the most relevant features of(photo)electrodes, with special emphasis on how to measure and optimize them. Finally, the review analyses the integration of(photo)electrodes in different photoelectrolyzer architectures, analyzing the most recent research work that comprises photocathode, photoanode,photocathode-photoanode, and tandem photoelectrolyzer configurations to ideally achieve self-sustained CO_(2) conversion systems. Overall, comprehensive guidelines are provided for future advancements in developing effective devices for CO_(2) conversion, bridging the gap towards the use of sunlight as the unique energy input and practical applications.展开更多
基金FAPESP,Brazil(#2023/10027-5,#2014/50945-4,#2020/15230-5,and#2021/000675-4)CNPq,Brazil(#465571/2014-0,#303269/2021-9,and#307837/2014-9)+6 种基金Instituto Serrapilheira(grant number Serra-2211-41925)FAPEMIG,Brazil(#PPM-00831-15)for support of this workCNPq,Brazil(#105944/2022-0)and PROPEUNESP(13/2022)FAPESP(#2019/00463-7,#2018/22845-6,and#2021/08007-0,respectively)for scholarshipsthe National Institute for Alternative Technologies of Detection,Toxicological Evaluation and Removal of Micropollutants and Radioactives(INCT-DATREM)the support of the Research Centre for Greenhouse Gas Innovation(RCGI),hosted by the University of Sao Paulo(USP)and sponsored by FAPESP and Shell Brasilthe strategic support given by ANP,Brazil(Brazilian National Oil,Natural Gas,and Biofuels Agency)through the R&D levy regulation。
文摘This work describes the use of TiO_(2)nanotubes-based electrodes(TNT)modified with Cu_(2)O nanostructures and gold nanoparticles for the photoelectroreduction of CO_(2)to produce value-added compounds.A thin layer of polydopamine was used as both an adherent agent and an electron transfer mediator,due to itsπ-conjugated electron system.The highest production yield was achieved using a TNT@PDA/Nc/Au40%electrode,with Faradaic efficiencies of 47.4%(110.5μM cm^(-2))and 27.8%(50.4μM cm^(-2))for methanol and methane,respectively.The performance of the photoelectrodes was shown to be Cu_(2)O facet-dependent,with cubic structures leading to greater conversion of CO_(2)to methanol(43%)and methane(27%),compared to the octahedral morphology,while a higher percentage of metallic gold on the nanostructured Cu_(2)O surface was mainly important for CH4production.Density functional theory(DFT)calculations supported these findings,attributing the superior photoelectrocatalytic performance of the TNT@PDA/Nc/Au40%electrode for CH4generation to the formation of an OCH3intermediate bonded to Au atoms.Studies using isotope-labeling and analysis by gas chromatograph-mass(GC-MS)demonstrated that13CO_(2)was the source for photoelectrocatalytic generation of13CH3OH and13CH313CH2OH.
基金the financial support received from the Spanish State Research Agency (AEI) through the projects PID2020-112845RB-I00, PID2019-104050RA-100, TED2021129810B-C21, and PLEC2022-009398 (MCIN/AEI/10.13039/50110 0011033 and Unión Europea Next Generation EU/PRTR)received funding from the European Union’s Horizon Europe research and innovation programme under grant agreement No 101118265the predoctoral research grant (FPI) PRE2021-097200。
文摘The photoelectrochemical conversion of CO_(2) into value-added products emerges as an attractive approach to alleviate climate change. One of the main challenges in deploying this technology is, however, the development and optimization of(photo)electrodes and photoelectrolyzers. This review focuses on the fabrication processes, structure, and characterization of(photo)electrodes, covering a wide range of fabrication techniques, from rudimentary to automated fabrication processes. The work also highlights the most relevant features of(photo)electrodes, with special emphasis on how to measure and optimize them. Finally, the review analyses the integration of(photo)electrodes in different photoelectrolyzer architectures, analyzing the most recent research work that comprises photocathode, photoanode,photocathode-photoanode, and tandem photoelectrolyzer configurations to ideally achieve self-sustained CO_(2) conversion systems. Overall, comprehensive guidelines are provided for future advancements in developing effective devices for CO_(2) conversion, bridging the gap towards the use of sunlight as the unique energy input and practical applications.
