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Artificial Photosynthesis for Carbon Dioxide Reduction and Conversion
摘要： In recent years, solar fuel or chemical production based on the photoreduction or fixation of CO2, the so-called “artificial photosynthesis” has received considerable attention. Thus, the development of an effective catalyst for the conversion of CO2 to useful organic molecules is desirable. Biocatalysts for CO2 reduction and conversion are useful catalyst for the artificial photosynthesis system. In this review, two types of artificial photosynthesis systems for CO2 reduction and conversion consisting of the visible-light sensitizer and biocatalyst are introduced. One is the artificial photosynthesis with visible-light sensitizer and biocatalyst for CO2 photoreduction to formic acid or methanol. The other one is the artificial photosynthesis with visible-light sensitizer, and novel electron carrier molecule and biocatalyst for the carbon-carbon bond formation from CO2 as a feedstock.
关键词： carbon-carbon bond formation,artificial photosynthesis,biocatalyst,CO2 reduction and conversion
更新于2025-09-23 15:23:52
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A four-state fluorescent molecular switch
摘要： Cross-coupling reactions are among the most powerful C–C and C–X bond forming tools in organic chemistry. Traditionally, cross-coupling methods rely on the use of aryl halides or pseudohalides as electrophiles. In the past three years, decarbonylative cross-couplings of amides have emerged as an attractive method for the construction of a wide variety of carbon–carbon and carbon–heteroatom bonds, allowing for the synthetically-valuable functional group inter-conversion of the amide bond. These previously elusive reactions hinge upon selective activation of the N–C(O) acyl amide bond, followed by CO extrusion, in a formal double N–C/C–C bond activation, to generate a versatile aryl–metal intermediate as an attractive alternative to traditional cross-couplings of aryl halides and pseudohalides. In this perspective review, we present recent advances and key developments in the field of decarbonylative cross-coupling reactions of amides as well as discuss future challenges and potential applications for this exciting field.
关键词： amides,transition-metal catalysis,C–C bond formation,decarbonylative cross-coupling,C–X bond formation
更新于2025-09-19 17:15:36
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[Topics in Organometallic Chemistry] || Functionalization of C(sp2)–H Bonds of Arenes and Heteroarenes Assisted by Photoredox Catalysts for the C–C Bond Formation
摘要： The formation of C–C bonds from arenes and heteroarenes through transition metal-catalyzed C–H bond functionalizations is one of the major achievements of these last decades. It is now possible to perform such transformations under mild reaction conditions with the help of visible light photocatalysis leading to eco-friendly and safer process to build organic molecules or materials. This chapter will focus on photoredox catalysis which involves a C(sp2)–H bond functionalization step for the formation of C(sp2)–C bonds [i.e., direct arylations and (per?uoro)alkylations] and will show how this hot topic contributes to the development of green chemistry.
关键词： MLTC photoredox catalysis,C(sp2)–H bond,Visible light,C–C bond formation
更新于2025-09-10 09:29:36
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Femtosecond X-ray solution scattering reveals that bond formation mechanism of a gold trimer complex is independent of excitation wavelength
摘要： The [Au(CN)2]3 trimer in water experiences a strong van der Waals interaction between the d10 gold atoms due to large relativistic effect and can serve as an excellent model system to study the bond formation process in real time. The trimer in the ground state (S0) exists as a bent structure without the covalent bond between the gold atoms, and upon the laser excitation, one electron in the antibonding orbital goes to the bonding orbital, thereby inducing the formation of a covalent bond between gold atoms. This process has been studied by various time-resolved techniques, and most of the interpretation on the structure and dynamics converge except that the structure of the first intermediate (S1) has been debated due to different interpretations between femtosecond optical spectroscopy and femtosecond X-ray solution scattering. Recently, the excitation wavelength of 267 nm employed in our previous scattering experiment was suggested as the culprit for misinterpretation. Here, we revisited this issue by performing femtosecond X-ray solution scattering with 310 nm excitation and compared the results with our previous study employing 267 nm excitation. The data show that a linear S1 structure is formed within 500 fs regardless of excitation wavelength and the structural dynamics observed at both excitation wavelengths are identical to each other within experimental errors.
关键词： bond formation mechanism,Femtosecond X-ray solution scattering,gold trimer complex,excitation wavelength
更新于2025-09-04 15:30:14
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Iodide Photoredox and Bond Formation Chemistry
摘要： Iodide redox chemistry is intimately coupled with the formation and breaking of chemical bonds that are relevant to emerging solar energy technologies. In this Account, recent advances in dye-sensitized iodide oxidation chemistry in organic solutions are described. Here RuII sensitizers with high cationic charge, tuned reduction potentials, and specific iodide receptor site(s) are shown to self-assemble in organic solvents and yield structures that rapidly oxidize iodide and generate I?I bonds when illuminated with visible light. These studies provided new insights into the fascinating behavior of our most polarizable and easily oxidized monatomic anion.
关键词： iodide,bond formation,RuII sensitizers,photoredox,solar energy
更新于2025-09-04 15:30:14