乙炔氢氯化反应中的负载金-离子液体催化剂: 离子态金物种的稳定机制

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

催化学报 ›› 2021, Vol. 42 ›› Issue (2): 334-346.DOI: 10.1016/S1872-2067(20)63617-8

乙炔氢氯化反应中的负载金-离子液体催化剂: 离子态金物种的稳定机制

赵佳^a^,^*(), 王赛赛^a, 王柏林^a^,^b, 岳玉学^a, 金春晓^a, 陆金跃^a, 方正^a, 庞祥雪^a, 丰枫^a, 郭伶伶^a, 潘志彦^b, 李小年^a^,^#()

^a浙江工业大学工业催化研究所, 浙江杭州310014
^b浙江工业大学环境工程学院, 浙江杭州310014

收稿日期:2020-03-21 接受日期:2020-05-10 出版日期:2021-02-18 发布日期:2021-01-21
通讯作者: 赵佳,李小年
基金资助:
国家自然科学基金(21606199);浙江省科技厅(LGG20B060004)

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

Jia Zhao^a^,^*(), Saisai Wang^a, Bolin Wang^a^,^b, Yuxue Yue^a, Chunxiao Jin^a, Jinyue Lu^a, Zheng Fang^a, Xiangxue Pang^a, Feng Feng^a, Lingling Guo^a, Zhiyan Pan^b, Xiaonian Li^a^,^#()

^aIndustrial Catalysis Institute of Zhejiang University of Technology, Hangzhou 310014, Zhejiang, China
^bDepartment of Environmental Engineering, Zhejiang University of Technology, Hangzhou 310014, Zhejiang, China

Received:2020-03-21 Accepted:2020-05-10 Online:2021-02-18 Published:2021-01-21
Contact: Jia Zhao,Xiaonian Li
About author:^#Tel: +86-571-88320002; E-mail: xnli@zjut.edu.cn
^*Tel: +86-571-88871656; E-mail: jiazhao@zjut.edu.cn;
Supported by:
National Natural Science Foundation of China(21606199);Science and Technology Department of Zhejiang Province is gratefully acknowledged(LGG20B060004)

摘要/Abstract

摘要：

聚氯乙烯(PVC)作为世界通用工程塑料之一, 具有优异的物理、化学和机械性能, 在工业、农业、建筑、包装、电力等行业中应用广泛. 氯乙烯是生产聚氯乙烯的重要单体. 氯乙烯的生产主要有电石法和乙烯法两种工艺路线, 由于我国“贫油、富煤、少气”的资源现状, 电石法产能占全部产能的83%以上. 电石法生产氯乙烯的原理是在氯化汞催化剂存在下, 将电石水解精制后的乙炔气与氯化氢加成直接合成氯乙烯. 随着节能减排及环保要求的逐渐提高和国际涉汞公约的实施, 开发新一代绿色无汞催化剂具有重要的战略意义. 近年来, 金基催化剂是无汞催化剂基础研究和技术开发中最重要的方向. 在之前的工作中, 我们课题组首先报道了负载离子液体-金催化剂体系(Au-SILP)在电石法生产氯乙烯工艺中的应用, 并发现离子液体的存在可以显著提高金活性物种在载体表面的分散度和稳定其化学价态. 在后续研究中, 我们在负载离子液体-金催化体系中引入金属铜离子(Cu²⁺), 利用反应过程中Au-Cu之间的氧化还原循环, 设计并制备了金属铜基配位离子液体, 构建了负载离子液体-金-铜催化剂体系. 铜离子的引入形成了一个催化剂自身维持氧化态的微环境, 实现了被还原金物种的原位氧化再生.
本文在上述研究基础上, 利用配位离子液体[Bmim][N(CN)₂]中[N(CN)₂^-]阴离子和阳离子金之间的强配位作用, 构建出比Au-Cl键更稳定的Au-N键, 并通过X射线光电子能谱(XPS)、球差校正-扫描透射电镜(AC-STEM)和扩展X射线吸收精细结构(EXAFS)表征证明了Au以单原子状态存在于载体表面. 制备的Au-N(CN)₂/AC催化剂在乙炔氢氯化反应中表现出比Au-Cl/AC和Au/AC催化剂更高的稳定性和催化活性以及更短的诱导期. 进一步表征分析发现, [N(CN)₂^-]配体促进了阳离子金和配体之间的电子转移, 提高了阳离子金的电子云密度, 削弱了乙炔在阳离子金上的吸附强度, 抑制了其还原, 提高了催化剂的稳定性. 更重要的是, 与阳离子金配位的[N(CN)₂^-]配体使得反应过程中的氯化氢在氮位点发生化学解离, 促进了氯化氢活化, 同时降低了反应能垒. 对负载配位离子液体-金催化体系反应诱导期的分析结果表明, 反应诱导期与反应物(乙炔、氯化氢)分子在离子液体层中的溶解度无关, 而主要取决于催化剂中Au(III)物种的含量和反应物分子在离子液体中的扩散速率. 上述研究结果进一步深化了离子液体和活性金物种之间电子的作用机理, 建立了负载离子液体-金催化剂体系对反应物的活化机制和反应机理, 为进一步开发具有工业应用价值的乙炔氢氯化反应无汞催化剂提供了科学基础和参考.

关键词: 乙炔氢氯化, 电子密度, 氯化氢活化, 稳定机理, 金基负载离子液体相催化剂

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

赵佳, 王赛赛, 王柏林, 岳玉学, 金春晓, 陆金跃, 方正, 庞祥雪, 丰枫, 郭伶伶, 潘志彦, 李小年. 乙炔氢氯化反应中的负载金-离子液体催化剂: 离子态金物种的稳定机制[J]. 催化学报, 2021, 42(2): 334-346.

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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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(20)63617-8

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

图/表 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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乙炔氢氯化反应中的负载金-离子液体催化剂: 离子态金物种的稳定机制

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

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