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Bromine and oxygen redox species mediated highly selective electro-epoxidation of styrene

Organic Chemistry Frontiers 2022年第2期9卷 436-444页

作者： Yuchi Zhang Asma Iqbal Jiantao Zai Shu-Yu Zhang Hongran Guo Xuejiao Liu Ibrahim ul Islam hira fazal Xuefeng Qian Shanghai Electrochemical Energy Devices Research Center School of Chemistry and Chemical Engineering and State Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong University Shanghai200240P.R.China

Olefin epoxidation is an essential transformation and arouses great interest among the scientific community for the key role of epoxide in the chemical industry.Traditional methods suffer from harmful oxidants and require harsh operating conditions and complex separation processes.Electro-epoxidation through bromine redox reactions is an eco-friendly strategy.However,the lack of efficient electrodes always limits the selectivity of epoxidation and results in massive energy consumption.Herein,we found that GF-CoS_(2)/CoS heterostructures anchored on graphite felt(GF-CoS_(2)/CoS)can efficiently facilitate the generation of bromine redox species on the anode.The synergistic cooperation between the bromine redox species and oxygen redox species(generated on a graphite rod cathode)can establish a benign electro-epoxidation system for olefin substrates in an ambient environment.Under the optimized reaction conditions,the epoxidation of styrene can achieve a yield of 97% at 30 mA cm^(-2).Importantly,the applied voltage(4-5 V)is roughly half of the Pt-based electrode system(7.8-9.3 V),hence,saving half of the energy.We demonstrated that our proposed strategy could also be applied to other olefins.Because of the simple,sustainable,and economic advantages of the epoxidation process,we believe this strategy is highly desirable for technical applications.

关键词： redox epoxidation styrene

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Copper vacancy activated plasmonic Cu3-xSnS4 for highly efficient photocatalytic hydrogen generation:Broad solar absorption,efficient charge separation and decreased HER overpotential

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Nano Research 2021年第10期14卷 3358-3364页

作者： Nazakat Ali Tsegaye Tadesse Tsega Yucai Cao Saghir Abbas Wenjing Li Asma Iqbal hira fazal Zhiling Xin Jiantao Zai Xuefeng Qian Shanghai Electrochemical Energy Devices Research Center School of Chemistry and Chemical Engineering and State Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Polyolefins and Catalysis Shanghai Key Laboratory of Catalysis Technology for Polyolefins(Shanghai Research Institute of Chemical Industry Co.Ltd.)Shanghai 200062China Shanghai Key Laboratory of Materials Protection and Advanced Materials in Electric Power Shanghai University of Electric Power2103 Pingliang RoadShanghai 200090China

Broad absorption spectra with efficient generation and separation of available charge carriers are indispensable requirements for promising semiconductor-based photocatalysts to achieve the ultimate goal of solar-to-fuel conversion.Here,Cu_(3-x)SnS_(4)(x=0-0.8)with copper vacancies have been prepared and fabricated via solvothermal process.The obtained copper vacancy materials have extended light absorption from ultraviolet to near-infrared-II region for its significant plasmonic effects.Time-resolved photoluminescence shows that the vacancies can simultaneously optimize charge carrier dynamics to boost the generation of long-lived active electrons for photocatalytic reduction.Density functional theory calculations and electrochemical characterizations further revealed that copper vacancies in Cu_(3-x)SnS_(4)tend to enhance hydrogen’s adsorption energy with an obvious decrease in its H_(2)evolution reaction(HER)overpotential.Furthermore,without any loadings,the H_(2)production rate was measured to be 9.5 mmol·h^(-1)·g^(-1).The apparent quantum yield was measured to be 27%for wavelengthλ>380 nm.The solar energy conversion efficiency was measured to be 6.5%under visible-near infrared(vis-NIR)(λ>420 nm).

关键词： hydrogen evolution reaction photocatalysis Cu_(3-x)SnS_(4) copper vacancy plasmon

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