Self-reduction for the Synthesis of Co Supported on Hierarchically Porous Carbon for Selective Hydrogenation Reaction †

doi:10.7503/cjcu20190687

Abstract

Abstract:

A series of supported cobalt-based nanocatalysts were synthesized by a one-step self-reduction method using cobalt-based organic framework as precursor. The effect of self-reduction of carbonization on the catalytic performance of supported cobalt-based catalysts was studied. This method successfully controlled the hierarchically porous structure of supports and the size of cobalt nanoparticles. The prepared Co-based catalysts had high catalytic activity and product selectivity for selective hydrogenation of 1,3-butadiene. Specially, it was found that the catalyst carbonized at 600 ℃ contained a hierarchically porous structure with large surface area, and a uniform distribution of cobalt nanoparticles without obvious aggregation. Most importantly, the corresponding sample exhibited a rather low 100% conversion temperature at 60 ℃ for selective hydrogenation of 1,3-butadiene, but with butenes selectivity as high as 61%. This work provides a new strategy for the preparation of supported non-noble metal catalysts with high-performance for hydrogenation reactions.

Key words: Hierarchically porous structure, Catalyst, Non-noble metal, Metal organic framework, Selective hydrogenation

CLC Number:

O643.38
O611

TrendMD:

HE Xiaoke, LI Xiaoyun, WANG Zhao, HU Nian, DENG Zhao, CHEN Lihua, SU Baolian. Self-reduction for the Synthesis of Co Supported on Hierarchically Porous Carbon for Selective Hydrogenation Reaction ^†[J]. Chem. J. Chinese Universities, 2020, 41(4): 639.

Figures/Tables 6

Fig.1 PXRD and simulated XRD patterns(A), SEM image(B), the N2 adsorption-desorption isotherms(C) and TGA-DSC curves(D) of ZIF-67Inset of (C): the corresponding pore size distribution curve of ZIF-67.

Fig.2 PXRD patterns of Co-N/C-T samples

Fig.3 SEM images(A—H) and size distributions(I—L) of Co-N/C-550(A, E, I), Co-N/C-600(B, F, J), Co-N/C-700(C, G, K) and Co-N/C-800(D, H, L)

Fig.4 N2 adsorption-desorption isotherms(A) and pore diameter distribution(B) of Co-N/C-T nanoparticles

Sample	$S a BET$ /(m²·g^-1)	$S b micro$ /(m²·g^-1)	$V c tol$ /(cm³·g^-1)	$V d micro$ /(cm³·g^-1)	Pore size/nm
ZIF-67	1755	1728	0.72	0.70	1.00, 1.48
Co-N/C-550	185	175	0.14	0.07	0.34, 0.47
Co-N/C-600	322	284	0.14	0.08	0.34, 0.47, 1.76, 3.90
Co-N/C-700	321	214	0.19	0.11	0.47, 1.57, 3.90
Co-N/C-800	313	147	0.21	0.06	0.59, 1.86, 4.00

Sample	$S a BET$ /(m²·g^-1)	$S b micro$ /(m²·g^-1)	$V c tol$ /(cm³·g^-1)	$V d micro$ /(cm³·g^-1)	Pore size/nm
ZIF-67	1755	1728	0.72	0.70	1.00, 1.48
Co-N/C-550	185	175	0.14	0.07	0.34, 0.47
Co-N/C-600	322	284	0.14	0.08	0.34, 0.47, 1.76, 3.90
Co-N/C-700	321	214	0.19	0.11	0.47, 1.57, 3.90
Co-N/C-800	313	147	0.21	0.06	0.59, 1.86, 4.00

Fig.5 Evolution of 1,3-butadiene conversion with the increase of reaction temperature(A) and selectivity to butenes with the butadiene conversion(B) of Co-N/C-T catalysts

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