For electrocatalytic water splitting, the sluggish anodic oxygen evolution reaction (OER) restricts the cathodic hydrogen evolution reaction (HER). Therefore, developing an alternative anodic reaction with accelerating kinetics to produce value-added chemicals, especially coupled with HER, is of great importance. Now, a thermodynamically more favorable primary amine (-CH -NH ) electrooxidation catalyzed by NiSe nanorod arrays in water is reported to replace OER for enhancing HER. The increased H production can be obtained at cathode; meanwhile, a variety of aromatic and aliphatic primary amines are selectively electrooxidized to nitriles with good yields at the anode. Mechanistic investigations suggest that Ni /Ni may serve as the redox active species for the primary amines transformation. Hydrophobic nitrile products can readily escape from aqueous electrolyte/electrode interface, avoiding the deactivation of the catalyst and thus contributing to continuous gram-scale synthesis.
Oxygen-containing and amino groups functionalized polymeric carbon nitride atomically-thin porous nanosheets with hydrophilic surfaces and strong Lewis basicity are designed and synthesized for enhanced photocatalytic H2evolution.
The development of efficient and low‐cost electrocatalysts toward the oxygen evolution reaction (OER) is critical for improving the efficiency of several electrochemical energy conversion and storage devices. Here, we report an elaborate design and synthesis of porous Co‐based trimetallic spinel oxide nanoboxes (NiCo2−xFexO4 NBs) by a novel metal‐organic framework engaged strategy, which involves chemical etching, cation exchange, and subsequent thermal oxidation processes. Owing to the structural and compositional advantages, the optimized trimetallic NiCo2−xFexO4 NBs (x is about 0.117) deliver superior electrocatalytic performance for OER with an overpotential of 274 mV at 10 mA cm−2, a small Tafel slope of 42 mV dec−1, and good stability in alkaline electrolyte, which is much better than that of Co‐based bi/monometallic spinel oxides and even commercial RuO2.
We present a convenient chemical conversion strategy for the synthesis of CoP porous ultrathin nanosheets as highly efficient catalysts for the hydrogen evolution reaction.
The unique optoelectronic properties and promising photovoltaic applications of organolead halide perovskites have driven the exploration of facile strategies to synthesize organometal halide perovskites and corresponding hybrid materials and devices. Currently, the preparation of CH3 NH3 PbBr3 perovskite nanowires, especially those with porous features, is still a great challenge. An efficient self-template-directed synthesis of high-quality porous CH3 NH3 PbBr3 perovskite nanowires in solution at room temperature using the Pb-containing precursor nanowires as both the sacrificial template and the Pb(2+) source in the presence of CH3 NH3 Br and HBr is now presented. The initial formation of CH3 NH3 PbBr3 perovskite layers on the surface of the precursor nanowires and the following dissolution of the organic component of the latter led to the formation of mesopores and the preservation of the 1D morphology. Furthermore, the perovskite nanowires are potential materials for visible-light photodetectors with high sensitivity and stability.
Confining nanostructured electrode materials in porous carbon represents an effective strategy for improving the electrochemical performance of lithium-ion batteries. Herein, we report the design and synthesis of hybrid hollow nanostructures composed of highly dispersed Co 3 O 4 hollow nanoparticles (sub-20 nm) embedded in the mesoporous walls of carbon nanoboxes (denoted as H-Co 3 O 4 @MCNBs) as an anode material for lithium-ion batteries. The facile metalorganic framework (MOF)-engaged strategy for the synthesis of H-Co 3 O 4 @MCNBs involves chemical etching-coordination and subsequent two-step annealing treatments. Owing to the unique structural merits including more active interfacial sites, effectively alleviated volume variation, good and stable electrical contact, and easy access of Li + ions, the H-Co 3 O 4 @MCNBs exhibit excellent lithium-storage performance in terms of high specific capacity, excellent rate capability, and cycling stability.
All‐inorganic semiconductor perovskite quantum dots (QDs) with outstanding optoelectronic properties have already been extensively investigated and implemented in various applications. However, great challenges exist for the fabrication of nanodevices including toxicity, fast anion‐exchange reactions, and unsatisfactory stability. Here, the ultrathin, core–shell structured SiO2 coated Mn2+ doped CsPbX3 (X = Br, Cl) QDs are prepared via one facile reverse microemulsion method at room temperature. By incorporation of a multibranched capping ligand of trioctylphosphine oxide, it is found that the breakage of the CsPbMnX3 core QDs contributed from the hydrolysis of silane could be effectively blocked. The thickness of silica shell can be well‐controlled within 2 nm, which gives the CsPbMnX3@SiO2 QDs a high quantum yield of 50.5% and improves thermostability and water resistance. Moreover, the mixture of CsPbBr3 QDs with green emission and CsPbMnX3@SiO2 QDs with yellow emission presents no ion exchange effect and provides white light emission. As a result, a white light‐emitting diode (LED) is successfully prepared by the combination of a blue on‐chip LED device and the above perovskite mixture. The as‐prepared white LED displays a high luminous efficiency of 68.4 lm W−1 and a high color‐rendering index of Ra = 91, demonstrating their broad future applications in solid‐state lighting fields.
Azoxy-, azo- and amino-aromatics are among the most widely used building blocks in materials science pharmaceuticals and synthetic chemistry, but their controllable and green synthesis has not yet been well established. Herein, a facile potential-tuned electrosynthesis of azoxy-, azo- and amino-aromatics via aqueous selective reduction of nitroarene feedstocks over a CoP nanosheet cathode is developed. A series of azoxy-, azo- and amino-compounds with excellent selectivity, good functional group tolerance and high yields are produced by applying different bias input. The synthetically significant and challenging asymmetric azoxy-aromatics can be controllably synthesized in moderate to good yields. The use of water as the hydrogen source makes this strategy remarkably fascinating and promising. In addition, deuterated aromatic amines with a high deuterium content can be readily obtained by using D2O. By pairing with anodic oxidation of aliphatic amines to nitriles, synthetically useful building blocks can be simultaneously produced in a CoP||Ni2P two-electrode electrolyzer. Only 1.25 V is required to achieve a current density of 20 mA cm−2, which is much lower than that of overall water splitting (1.70 V). The paired oxidation and reduction reactions can also be driven using a 1.5 V battery to synthesize nitrile and azoxybenzene with good yields and selectivity, further emphasizing the flexibility and controllability of our method. This work paves the way for a promising approach to the green synthesis of valuable chemicals through potential-controlled electrosynthesis.
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