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RSC Advances · 2016 ·Vol. 6 ·期 35 ·29638-29645 · IF 3.289

Combined experimental/theoretical study of D-glucosamine promoted Ullmann-type C–N coupling catalyzed by copper(I): does amino really count?

Xin Ge,Xinzhi Chen,Chao Qian,Shaodong Zhou

Ullmann type C–N coupling reaction catalyzed by copper(I) with D-glucosamine derivatives as promoters was studied by means of combined experimental/theoretical investigation. The catalytic role of D-glucosamine was addressed. In contrast with previous speculations, the amino group may not count in the catalytic cycle in which the oxidative addition/reductive elimination mechanism works. Experimental results are in good agreement with theoretical findings. Extensive work indicates the wide applicability of the C–N coupling strategy exploited in this work.

研究领域: 有机化学 · 催化化学 · 药物化学 · 计算化学 · 合成方法学 · 生物正交化学 · 金属有机化学

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CHINESE JOURNAL OF CATALYSIS · 2021 ·Vol. 42 ·期 10 ·1798-1807 · IF 8.271

Controlling atomic phosphorous-mounting surfaces of ultrafine W2C nanoislands monodispersed on the carbon frameworks for enhanced hydrogen evolution

Xiangyong Zhang,Tianying Liu,Ting Guo,Xueying Han,Zongyun Mu,Qiang Chen,Jiangmin Jiang,Jing Yan,Jiaren Yuan,Dezhi Wang,Zhuangzhi Wu,Zongkui Kou

Controllably mounting foreign atoms on the surfaces of earth-abundant electrocatalysts strongly improve their surface electronic properties for optimizing the catalytic performance of surficial sites to an unusual level, and provides a good platform to gain deep insights into catalytic reactions . The present work describes, employing ultrafine W 2 C nanoislands (average size: 2.3 nm) monodispersed on the N, P dual-doped carbon frameworks as a model system, how to regulate the atomic phosphorous-mounting effect on the surfaces of W 2 C to derive an active and stable P-mounting W 2 C (WCP) catalyst for both acidic and alkaline hydrogen evolution reaction (HER). Since in situ phosphorus substitution into carbon sites of preformed W 2 C nanoislands gradually proceeds from surfaces to solids, so that using a proper amount of phosphorus sources can readily control the surface mounting level to avoid the mass P-doping into the bulk. By this way, the activity per active site of WCP catalyst with robust stability can be optimized to 0.07 and 0.56 H 2 s −1 at –200 mV overpotential in acid and base, respectively, which reach up to the several-fold of pure-phase W 2 C (0.01 and 0.05 H 2 s −1 ). Theoretical investigations suggest that compared with solid P doping, the P mounting on W 2 C surface can more remarkably enhance its metallicity and decrease the hydrogen release barrier. This finding disclosed a key correlation between surface foreign atom-mounting and catalytic activity , and suggested a logical extension to other earth-abundant catalysts for various catalytic reactions .

研究领域: 材料化学 · 电催化 · 纳米材料 · 能源科学 · 表面科学 · 理论计算

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Combined experimental/theoretical study of D-glucosamine promoted Ullmann-type C–N coupling catalyzed by copper(I): does amino really count?

Controlling atomic phosphorous-mounting surfaces of ultrafine W2C nanoislands monodispersed on the carbon frameworks for enhanced hydrogen evolution