The electrochemical oxygen evolution reaction (OER) is an essential anodic reaction that converts sustainable energy into chemical fuels, as it can provide protons and electrons. One of the most challenging research directions for the practical application of the OER is the elevation of the activity of noble-metal-free electrocatalysts. Here, we report that the nickel foam can be used as an electron-deficient substrate to tune the surface oxidation state of catalytic electrodes and thus boost the OER activity of CuP nanosheets via a charge-storage mechanism.
View Article and Find Full Text PDFPlatinum (Pt) is the most effective bench-marked catalyst for producing renewable and clean hydrogen energy by electrochemical water splitting. There is demand for high HER catalytic activity to achieve efficient utilization and minimize the loading of Pt in catalysts. In this work, we significantly boost the HER mass activity of Pt nanoparticles in Pt /Co to 8.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2021
NO reduction acts a pivotal part in sustaining globally balanced nitrogen cycle and restoring ecological environment, ammonia (NH ) is an excellent energy carrier and the most valuable product among all the products of NO reduction reaction, the selectivity of which is far from satisfaction due to the intrinsic complexity of multiple-electron NO -to-NH process. Here, we utilize the Schottky barrier-induced surface electric field, by the construction of high density of electron-deficient Ni nanoparticles inside nitrogen-rich carbons, to facilitate the enrichment and fixation of all NO anions on the electrode surface, including NO and NO , and thus ensure the final selectivity to NH . Both theoretical and experimental results demonstrate that NO anions were continuously captured by the electrode with largely enhanced surface electric field, providing excellent Faradaic efficiency of 99 % from both electrocatalytic NO and NO reduction.
View Article and Find Full Text PDFThe activation of C-H bonds is a central challenge in organic chemistry and usually a key step for the retro-synthesis of functional natural products due to the high chemical stability of C-H bonds. Electrochemical methods are a powerful alternative for C-H activation, but this approach usually requires high overpotential and homogeneous mediators. Here, we design electron-deficient WC nanocrystal-based electrodes to boost the heterogeneous activation of C-H bonds under mild conditions via an additive-free, purely heterogeneous electrocatalytic strategy.
View Article and Find Full Text PDFProduction of ammonia is currently realized by the Haber-Bosch process, while electrochemical N fixation under ambient conditions is recognized as a promising green substitution in the near future. A lack of efficient electrocatalysts remains the primary hurdle for the initiation of potential electrocatalytic synthesis of ammonia. For cheaper metals, such as copper, limited progress has been made to date.
View Article and Find Full Text PDFA nitrogen-thermal approach via the reaction between transition metal species and N dopants affords us the ability to optimize the tradeoff between the number of exposed transition metal/carbon (exemplified by cobalt in this work) boundaries and the most pronounced interfacial rectifying contact to achieve the highly efficient and selective hydrogenation and dehydrogenation of N-heterocycle compounds in a reversible manner.
View Article and Find Full Text PDFHighly efficient fixation of CO for the synthesis of useful organic carbonates has drawn much attention. The design of sustainable Lewis acid-base pairs, which has mainly relied on expensive organic ligands, is the key challenge in the activation of the substrate and CO molecule. Here, we report the application of Mott-Schottky type nanohybrids composed of electron-deficient Cu and electron-rich N-doped carbon for CO fixation.
View Article and Find Full Text PDFThe exploitation of metal-free organic polymers as electrodes for water splitting reactions is limited by their presumably low activity and poor stability, especially for the oxygen evolution reaction (OER) under more critical conditions. Now, the thickness of a cheap and robust polymer, poly(p-phenylene pyromellitimide) (PPPI) was rationally engineered by an in situ polymerization method to make the metal-free polymer available for the first time as flexible, tailorable, efficient, and ultra-stable electrodes for water oxidation over a wide pH range. The PPPI electrode with an optimized thickness of about 200 nm provided a current density of 32.
View Article and Find Full Text PDFEngineering the adsorption of molecules on active sites is an integral and challenging part for the design of highly efficient transition-metal-based catalysts for methanol dehydrogenation. A Mott-Schottky catalyst composed of Ni nanoparticles and tailorable nitrogen-doped carbon-foam (Ni/NCF) and thus tunable adsorption energy is presented for highly efficient and selective dehydrogenation of gas-phase methanol to hydrogen and CO even under relatively high weight hourly space velocities (WHSV). Both theoretical and experimental results reveal the key role of the rectifying contact at the Ni/NCF boundaries in tailoring the electron density of Ni species and enhancing the absorption energies of methanol molecules, which leads to a remarkably high turnover frequency (TOF) value (356 mol methanol mol Ni h at 350 °C), outpacing previously reported bench-marked transition-metal catalysts 10-fold.
View Article and Find Full Text PDFIn this paper, coenzyme Q10 (Ubiquinone, CoQ10) was used for the first time as a transducer to construct electrochemical biosensor for effectively detecting γ-L-glutamyl-L-cysteinyl-glycine (glutathione, GSH). CoQ10 modified electrode was fabricated by attaching its gel mixed with multi-walled carbon nanotubes (MWNTs)/ionic liquid (IL). In the optimum conditions, based on the increasing of reduction peak current of CoQ10 caused by GSH through voltammetric technology, it was found that the peak current of CoQ10 was linear with the concentration of GSH in the range from 4.
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