We report a catalyst made of Pd nanoparticles (NPs) supported on mesoporous N-doped carbon, Pd@CN(0132), which was shown to be highly active in promoting biomass refining. The use of a task-specific ionic liquid (3-methyl-1-butylpyridine dicyanamide) as a precursor and silica NPs as a hard template afforded a high-nitrogen-content (12 wt %) mesoporous carbon material that showed high activity in stabilizing Pd NPs. The resulting Pd@CN(0.132) catalyst showed very high catalytic activity in hydrodeoxygenation of vanillin (a typical model compound of lignin) at low H(2) pressure under mild conditions in aqueous media. Excellent catalytic results (100% conversion of vanillin and 100% selectivity for 2-methoxy-4-methylphenol) were achieved, and no loss of catalytic activity was observed after six recycles.
ARTICLE
This journal isHierarchically porous carbons (HPCs) show great potentials in energy storage due to their high surface area as well as short ion transport path derived from the interconnected porous framework. However, most existing protocols highly rely on the nanocasting and soft -templating, which usually restrict the using of raw materials and thus industrial unfeasible. It still reminds a big challenge to build HPCs from crude biomass, which is abundant on the earth, through a simply one-pot approach. Inspired by leavening bread, we design a strategy to fabricate HPCs with three-dimensional (3D) hierarchical pores consisting of macro, meso, and micropores. The "leavening method" is conducted simply by mixing the biomass with KHCO3 followed by undergoing elevated temperature treatment. Besides the well-defined hierarchical structure, the as-prepared HPCs also exhibit notably large specific areas (up to 1893 m 2 g -1 ). It is noteworthy that this "leavening" strategy is widely applicable for most of biomass derivatives and biomass, including glucose, cellulose, chitin, starch, rice straw, bamboo, and etc. When evaluated as supercapacitor electrode materials in two-electrode test systems, the as-prepared HPCs exhibit an excellent electrochemical performance: specific capacitance of 253 F g -1 , almost no capacitance loss after 10 000 cycles.Scheme 1 Scheme diagram of the formation of Cx-LE: mixing the biomass with the "leavening" agents, followed by calcination under the insert gas for the synthesis of Cx-LE.A simple and universal methodology for carbon materials derived from biomass with hierarchical structure.
M
n+1
AX
n
phases are a large family of compounds that have been limited, so far, to carbides and nitrides. Here we report the prediction of a compound, Ti
2
InB
2
, a stable boron-based ternary phase in the Ti-In-B system, using a computational structure search strategy. This predicted Ti
2
InB
2
compound is successfully synthesized using a solid-state reaction route and its space group is confirmed as
P
m2
(No. 187), which is in fact a hexagonal subgroup of
P6
3
/mmc
(No. 194), the symmetry group of conventional M
n+1
AX
n
phases. Moreover, a strategy for the synthesis of MXenes from M
n+1
AX
n
phases is applied, and a layered boride, TiB, is obtained by the removal of the indium layer through dealloying of the parent Ti
2
InB
2
at high temperature under a high vacuum. We theoretically demonstrate that the TiB single layer exhibits superior potential as an anode material for Li/Na ion batteries than conventional carbide MXenes such as Ti
3
C
2
.
The development of efficient systems for selective aerobic oxidation of hydrocarbons and alcohols to produce more functional compounds (aldehydes, ketones, acids or esters) with atmospheric air or molecular oxygen is a grand challenge for the chemical industry. Here we report the synthesis of palladium nanoparticles supported on novel nanoporous nitrogendoped carbon, and their impressive performance in the controlled oxidation of hydrocarbons and alcohols with air. In terms of catalytic activity, these catalysts afford much higher turnover frequencies (up to 863 turnovers per hour for hydrocarbon oxidation and up to B210,000 turnovers per hour for alcohol oxidation) than most reported palladium catalysts under the same reaction conditions. This work provides great potential for the application of ambient air and recyclable palladium catalysts in fine-chemical production with high activity.
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