Controllable hydrogen release from NH3BH3 hydrolysis over Ru ultrafine particles stabilized on agriculture waste-derived carbon

Shi-Long Yang, Shi-Nuo Liu, Kang-Jian Dub,Xiu-Cheng Zheng,Zhi-Kun Peng,Pu Liu

COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS(2024)

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摘要
Simultaneously considering cost, safety and catalytic efficiency, the development of a cost-effective and highperformance catalyst is significant and challenging for controllable hydrogen release from ammonia borane (AB, NH3BH3) hydrolysis. In this work, Ru ultrafine particles are evenly and firmly stabilized on wheat straw derived porous carbon through a facile procedure. Specifically, attributed to the abundant co-doping of heteroatoms (namely, N and O) and suitable hierarchical porous structure of WSC-1.0 with large specific surface area (1000 m2 g-1), which is prepared with a mass ratio of 1: 1 for K2CO3 to the pre-carbonized biomass waste, as well as high dispersion (32.6%) of Ru ultrafine particles with an average size of 1.4 +/- 0.3 nm, the optimal Ru/ WSC-1.0 displays exceptional catalytic performance in the hydrolysis of AB. The corresponding turnover frequency (TOF) and specific reaction rate (rB) are 167.7 min- 1 and 4.07 x 104 mL min- 1 gRu- 1, respectively, and the apparent activation energy is 40.94 kJ mol-1. Upon adding NaOH (1.0 M), the hydrolysis rate can be remarkably accelerated (TOF = 401.4 min 1, rB = 9.75 x 104 mL min- 1 gRu-1). The isotope experiments show that the scission of an O-H bond in H2O by oxidative addition is the decisive step in this reaction. Impressively, the effective "on off" control for the hydrolytic dehydrogenation reaction over Ru/WSC-1.0 can be easily realized by introducing certain amounts of Zn(NO3)2 and EDTA-2Na, separately. Our work delivers a facile approach for efficient utilization of agricultural wastes and offers a robust and cost-effective catalyst for the controllable hydrogen evolution from AB hydrolysis.
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关键词
Wheat straws,N/O co-doping,Hierarchically porous carbon,Ru ultrafine particles,Hydrolysis of ammonia borane,Controllable hydrogen evolution
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