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Nate W. J. Ang Joo C. A. Oliveira Lutz Ackermann 《Angewandte Chemie (International ed. in English)》2020,59(31):12842-12847
The chemical use of CO2 as an inexpensive, nontoxic C1 synthon is of utmost topical interest in the context of carbon capture and utilization (CCU). We present the merger of cobalt catalysis and electrochemical synthesis for mild catalytic carboxylations of allylic chlorides with CO2. Styrylacetic acid derivatives were obtained with moderate to good yields and good functional group tolerance. The thus‐obtained products are useful as versatile synthons of γ‐arylbutyrolactones. Cyclic voltammetry and in operando kinetic analysis were performed to provide mechanistic insights into the electrocatalytic carboxylation with CO2. 相似文献
33.
Julien Warnan Erwin Reisner 《Angewandte Chemie (International ed. in English)》2020,59(40):17344-17354
From the understanding of biological processes and metalloenzymes to the development of inorganic catalysts, electro‐ and photocatalytic systems for fuel generation have evolved considerably during the last decades. Recently, organic and hybrid organic systems have emerged to challenge the classical inorganic structures through their enormous chemical diversity and modularity that led earlier to their success in organic (opto)electronics. This Minireview describes recent advances in the design of synthetic organic architectures and promising strategies toward (solar) fuel synthesis, highlighting progress on materials from organic ligands and chromophores to conjugated polymers and covalent organic frameworks. 相似文献
34.
Jinze Liu Yating Wang Hao Jiang Haibo Jiang Xiaodong Zhou Yuhang Li Chunzhong Li 《化学:亚洲杂志》2020,15(3):425-431
Electrochemical reduction of carbon dioxide (CO2) to CO is regarded as an efficient method to utilize the greenhouse gas CO2, because the CO product can be further converted into high value‐added chemicals via the Fisher–Tropsch process. Among all electrocatalysts used for CO2‐to‐CO reduction, Au‐based catalysts have been demonstrated to possess high selectivity, but their precious price limits their future large‐scale applications. Thus, simultaneously achieving high selectivity and reasonable price is of great importance for the development of Au‐based catalysts. Here, we report Ag@Au core–shell nanowires as electrocatalyst for CO2 reduction, in which a nanometer‐thick Au film is uniformly deposited on the core Ag nanowire. Importantly, the Ag@Au catalyst with a relative low Au content can drive CO generation with nearly 100 % Faraday efficiency in 0.1 m KCl electrolyte at an overpotential of ca. ?1.0 V. This high selectivity of CO2 reduction could be attributed to a suitable adsorption strength for the key intermediate on Au film together with the synergistic effects between the Au shell and Ag core and the strong interaction between CO2 and Cl? ions in the electrolyte, which may further pave the way for the development of high‐efficiency electrocatalysts for CO2 reduction. 相似文献
35.
Guangmei Cai Lihua Zeng Lanqi He Shujian Sun Yexiang Tong Jianyong Zhang 《化学:亚洲杂志》2020,15(13):1963-1969
A series of porphyrin‐based imine gels have been synthesized via dynamic covalent gelation between 5,10,15,20‐tetra(4‐aminophenyl)‐21H,23H‐porphyrin (H2TAPP) derivatives and various aldehyde compounds. The porphyrin‐ferrocene imine gels based on MTAPP (M=H2, Ni2+, Co2+, Pd2+ and Zn2+) and ferrocene‐1,1′‐dicarbaldehyde (NA) display efficient HER, OER and ORR activities in alkaline media. Among the gels, CoTAPP‐NA shows an HER current density of 10 mA cm?2 at low overpotential of 470 mV and small Tafel slope of 110 mV decade?1 in alkaline media. CoTAPP‐NA also exhibits OER catalytic activity with low overpotential (416 mV for 10 mA cm?2). CoTAPP‐NA shows ability in overall water splitting in alkaline media. In addition, CoTAPP‐NA exhibits onset potential (Ep) of 0.95 V and half‐wave potential (E1/2) of 0.84 V in 1.0 mol L?1 KOH solution for oxygen reduction. Moreover, the gel catalyst shows good stability. 相似文献
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A polymer film of tetra(p-aminophenyl) porphyrin nickel was obtained at a glassy carbon electrode by a cyclic voltammetric method. Cyclic voltammograms of the film electrode exhibited two stable redox waves with anodic peak potential at 0.43V and cathodic peak potential at 0.30 V in 0.5M NaOH aqueous solution. The electrocatalytic characteristics of the film electrode were studied by cyclic voltammetry, a. c. impedance analysis and other methods. The oxidation peak current increased linearly with the addition of acetaminophen to the aqueous NaOH medium in the range 1 × 10–6–2 × 10–4
M acetaminophen. The performance of the electrode was verified by the determination of acetaminophen in a paracetamol preparation. 相似文献
38.
聚中性红膜修饰电极测定痕量NO2^—的研究 总被引:4,自引:1,他引:4
研究了聚中性红膜修饰电极对NO-2的催化氧化性能,建立了测定NO-2的新方法。NO-2的浓度在2.0×10-6~5.0×10-3mol/L范围内与催化氧化峰电流呈良好的线性关系,检测限为6.0×10-7mol/L。若利用计时电流法分析,检测限可达8.0×10-8mol/L。 相似文献
39.
应用电化学法聚合酚藏花红(PPS)功能化的单壁碳纳米管,以其作为烟酰胺辅酶(NADH)氧化的电化学催化剂(电极),构建基于乙醇脱氢酶的安培型乙醇生物电化学传感器.该电极于0.0 V时,对NADH具有很好的催化性能.而单体酚藏花红则由于其电位过低(-0.48 V),不能显示催化性能.循环伏安和计时安培法测试表明:该传感器... 相似文献
40.
Cobalt‐Embedded Nitrogen‐Rich Carbon Nanotubes Efficiently Catalyze Hydrogen Evolution Reaction at All pH Values 下载免费PDF全文
Dr. Xiaoxin Zou Xiaoxi Huang Dr. Anandarup Goswami Dr. Rafael Silva Dr. Bhaskar R. Sathe Eliška Mikmeková Prof. Tewodros Asefa 《Angewandte Chemie (International ed. in English)》2014,53(17):4372-4376
Despite being technically possible, splitting water to generate hydrogen is still practically unfeasible due mainly to the lack of sustainable and efficient catalysts for the half reactions involved. Herein we report the synthesis of cobalt‐embedded nitrogen‐rich carbon nanotubes (NRCNTs) that 1) can efficiently electrocatalyze the hydrogen evolution reaction (HER) with activities close to that of Pt and 2) function well under acidic, neutral or basic media alike, allowing them to be coupled with the best available oxygen‐evolving catalysts—which also play crucial roles in the overall water‐splitting reaction. The materials are synthesized by a simple, easily scalable synthetic route involving thermal treatment of Co2+‐embedded graphitic carbon nitride derived from inexpensive starting materials (dicyandiamide and CoCl2). The materials’ efficient catalytic activity is mainly attributed to their nitrogen dopants and concomitant structural defects. 相似文献