Acetylene hydrochlorination over supported ionic liquid phase (SILP) gold-based catalyst: Stabilization of cationic Au species via chemical activation of hydrogen chloride and corresponding mechanisms

doi:10.1016/S1872-2067(20)63617-8

Abstract

Abstract:

The activation of HCl by cationic Au in the presence of C₂H₂ is important for the construction of active Au sites and in acetylene hydrochlorination. Here, we report a strategy for activating HCl by the Au-based supported ionic liquid phase (Au-SILP) technology with the [N(CN)₂^-] anion. This strategy enables HCl to accept electrons from [N(CN)₂^-] anions in Au-[N(CN)₂^-] complexes rather than from pure [Bmim][N(CN)₂], leading to notable improvement in both the reaction path and the stability of the catalyst without changing the reaction triggered by acetylene adsorption. Furthermore, the induction period of the Au-SILP catalyst was shown to be absent in the reaction process due to the high Au(III) content in the Au(III)/Au(I) site and the high substrate diffusion rate in the ionic liquid layer. This work provides a facile method to improve the stability of Au-based catalysts for acetylene hydrochlorination.

Key words: Acetylene hydrochlorination, Electron density, Hydrogen chloride activation, Stabilization mechanism, Gold-based supported ionic liquid, phase catalyst

Jia Zhao, Saisai Wang, Bolin Wang, Yuxue Yue, Chunxiao Jin, Jinyue Lu, Zheng Fang, Xiangxue Pang, Feng Feng, Lingling Guo, Zhiyan Pan, Xiaonian Li. Acetylene hydrochlorination over supported ionic liquid phase (SILP) gold-based catalyst: Stabilization of cationic Au species via chemical activation of hydrogen chloride and corresponding mechanisms[J]. Chinese Journal of Catalysis, 2021, 42(2): 334-346.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63617-8

https://www.cjcatal.com/EN/Y2021/V42/I2/334

Figures/Tables 12

Fig. 1. Characterizations of the Au-N(CN)2/AC catalyst. (a) N2 gas adsorption/desorption isotherms; (b) STEM image and elemental mapping analysis; (c) XRD patterns; (d) representative HAADF-STEM image and (e) Au 4f XPS spectra.

Table 1 Textural properties of the AC support and Au-SILP catalysts.

Sample	S_BET (m² g^-1) ^a	Volume (cm³ g^-1) ^b	Diameter (nm) ^c
Au-N(CN)₂/AC	722	0.39	2.01
Au-Cl/AC	737	0.40	2.04
AC	1135	0.64	2.20

Table 2 EXAFS fitting parameters at the Au L3-edge for Au-N(CN)2/AC and Au-Cl/AC catalysts.

Sample	Scattering path	CN ^a	R (Å) ^b	σ² (Å²) ^c	ΔE₀ (eV) ^d	R factor
Au foil	Au-Au	12	2.86	0.0079	3.9	0.004
KAuCl₄	Au-Cl	3.9	2.27	0.0024	9.2	0.018
(PPh₃)AuCH₃	Au-P	1.7	2.28	0.0032	2.4	0.008
(PPh₃)AuCH₃	Au-C	1.0	2.05	0.0032	2.4	0.008
Au-Cl/AC	Au-Cl	3.0	2.27	0.0012	8.3	0.014
Au-Cl/AC	Au-Au	0.5	2.86	0.0012	8.3	0.014
Au-N(CN)₂/AC	Au-Cl	1.4	2.27	0.0013	2.0	0.019
Au-N(CN)₂/AC	Au-N	5.3	3.22	0.0013	2.0	0.019

Fig. 2. The edge-normalized XANES spectra at the Au L3-edge for the Au-N(CN)2/AC and Au-Cl/AC catalysts and reference Au samples. (a) White line intensity and (b) R-space.

Fig. 3. VCM productivity as a function of (a) time on stream, h, and at GHSV(C2H2) = 1000 h-1; (b) VCM productivity versus the GHSV and Au loading for the investigated Au-N(CN)2/AC; (c) apparent activation energies of the Au-Cl/AC and Au-N(CN)2/AC catalysts; (d) VCM productivity of Au-N(CN)2/AC and other Au-based catalysts reported in literature. Numbers 11-13 indicate the productivity of the Au-N(CN)2/AC catalyst at different GHSV(C2H2) values; (e) VCM productivity as a function of the deactivation rate for various samples.

Fig. 4. Optimized structures of (a) [Bmim][Cl], (b) C2H2-[Bmim][Cl], (c) HCl-[Bmim][Cl], (d) [Bmim][N(CN)2], (e) C2H2-[Bmim][N(CN)2], and (f) HCl-[Bmim][N(CN)2]. The dotted lines represent the possible modes of interaction, with interatomic distances in angstroms. The solubilities of (g) C2H2 and (h) HCl in the investigated [Bmim][Cl] and [Bmim][N(CN)2] ILs at different temperatures; (i) diffusion coefficients for C2H2 and HCl in [Bmim][Cl] and [Bmim][N(CN)2]. Color code: H, white; C, gray; N, blue; Cl, light green.

Fig. 5. Characterizations of the spent (a,c) Au-Cl/AC and (b,d) Au-N(CN)2/AC catalysts. (a,b) TEM images; (c,d) XPS results.

Table 3 Porous structure and metal content of the spent Au-based catalysts.

Sample	S_BET (m² g^-1)^a	Volume (cm³ g^-1) ^b	Au content (wt%) ^c
Spent Au-N(CN)₂/AC	695	0.38	0.09
Spent Au-Cl/AC	787	0.37	0.11

Fig. 6. (a) Electron density and (b) the Hirshfeld charge of the Au atoms in various Au states.

Fig. 7. Reaction pathways of the Au-Cl/AC and Au-N(CN)2/AC catalysts.

Fig. 8. Hirshfeld charge of the N atoms before and after HCl adsorption. (a) AuCl3-[Bmim][N(CN)2]; (b) [Bmim][N(CN)2].

Fig. 9. Scheme 1. Schematic representation of the Au-N(CN)2/AC catalyst. The image is not drawn to scale.

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