The development of effective and inexpensive catalysts for hydrogen release from hydrogen-storage compounds such as ammonia-borane (AB) is crucial in academic and industrial fields for the reduction of greenhouse gas emissions . Herein, we report a facile method to fabricate well-dispersed CoP nanoparticles (NPs) with an average particle size of 4.3 nm. The CoP NPs were encapsulated in carbonaceous nanorods (CoP@CNR) using metal-organic frameworks (MOFs) as a sacrificial precursor. The CoP@CNR catalysts were characterized, and their catalytic performance for the dehydrogenization of AB at 25 °C in an alkaline solution was determined. CoP@CNR (400) with a hierarchically meso-microporous structure (micropore area = 73.6 m 2 g -1 and micropore volume = 0.19 cm 3 g -1 ) and a specific surface area of 88.4 m 2 g -1 was synthesized during the phosphorization process. The hierarchically porous structure was instrumental in immobilizing metal NPs and accelerating mass diffusion. Moreover, the incorporation of P into Co NPs modified the electronic structure of the latter and accelerated the dehydrogenization of AB. This resulted in a hydrogen release rate of 10,014 mL/(min·g), which was 13 times higher than that of the pure Co nanocatalyst. In addition, we reported the kinetic studies for AB hydrolysis catalyzed by CoP@CNR (400) in terms of the temperature effect, isotope effect , catalyst concentration, AB concentration, and NaOH concentration.
A dehydrogenative C(sp2)–N bond-forming strategy via copper-catalyzed intramolecular C–H/N–H coupling has been developed, which systematically unraveled the feasibility and practicality for benzoimdazo[1,2-a]indole formations through oxidative anilidic N–H activation. The merit of this strategy is illustrated by the broad tolerance of functionalities, as well as the utilization of extremely cheap copper catalysis to realize potentially useful indole-fused tetracycles in a step- and atom-economical manner.
Simultaneous generation of H 2 fuel and value-added chemicals has attracted increasing attention since the photogenerated electrons and holes can be both employed to convert solar light into chemical energy. Herein, for realizing UV-visible-NIR light driven dehydrogenation of benzyl alcohol (BA) into benzaldehydes (BAD) and H 2 , a novel localized surface plasmon resonance (LSPR) enhanced S-scheme heterojunction was designed by combining noble-metal-free plasmon MoO 3– x as oxidation semiconductor and Zn 0.1 Cd 0.9 S as reduction semiconductor. The photoredox system of Zn 0.1 Cd 0.9 S/MoO 3– x displayed an unconventional reaction model, in which the BA served as both electron donor and acceptor. The S-scheme charge transfer mechanism induced by the formed internal electric field enhanced the redox ability of charge carriers thermodynamically and boosted charge separation kinetically. Moreover, due to the LSPR effect of MoO 3− x nanosheets , Zn 0.1 Cd 0.9 S/MoO 3− x photocatalysts exhibited strong absorption in the region of full solar spectrum. Therefore, the Zn 0.1 Cd 0.9 S/MoO 3− x composite generated H 2 and BAD simultaneously via selective oxidation of BA with high production (34.38 and 33.83 mmol·g −1 for H 2 and BAD, respectively) upon full solar illumination. Even under NIR light irradiation, the H 2 production rate could up to 94.5 mmol·g −1 ·h −1 . In addition, the Zn 0.1 Cd 0.9 S/MoO 3– x composite displayed effective photocatalytic H 2 evolution rate up to 149.2 mmol·g −1 ·h −1 from water, which was approximate 6 times that of pure Zn 0.1 Cd 0.9 S. This work provides a reference for rational design of plasmonic S-scheme heterojunction photocatalysts for coproduction of high-value chemicals and solar fuel production.
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