乙炔氢氯化非金属碳催化剂的研究进展: 从杂原子掺杂到本征缺陷

doi:10.1016/S1872-2067(24)60245-7

催化学报 ›› 2025, Vol. 70: 8-43.DOI: 10.1016/S1872-2067(24)60245-7

乙炔氢氯化非金属碳催化剂的研究进展: 从杂原子掺杂到本征缺陷

魏抒豪, 蓝国钧^*(), 邱一洋, 林迪, 孔薇, 李瑛^*()

浙江工业大学化工学院, 工业催化研究所, 浙江杭州 310014

收稿日期:2025-01-19 接受日期:2025-02-14 出版日期:2025-03-18 发布日期:2025-03-20
通讯作者: * 电子信箱: liying@zjut.edu.cn (李瑛),languojun@zjut.edu.cn (蓝国钧).
基金资助:
国家重点研发计划(2024YFC3907904);国家自然科学基金企业创新发展联合基金(U23B20162)

Advances in metal-free carbon catalysts for acetylene hydrochlorination: From heteroatom doping to intrinsic defects over the past decade

Shuhao Wei, Guojun Lan^*(), Yiyang Qiu, Di Lin, Wei Kong, Ying Li^*()

Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou310014, Zhejiang, China

Received:2025-01-19 Accepted:2025-02-14 Online:2025-03-18 Published:2025-03-20
Contact: * E-mail: liying@zjut.edu.cn (Y. Li),languojun@zjut.edu.cn (G. Lan).
About author:Guojun Lan (Institute of Industrial catalysis, College of Chemical Engineering, Zhejiang University of Technology) received his B. Sc., and PhD degree from Zhejiang University of Technology in 2010 and 2016, respectively. During the period from January 2013 to August 2015, he was jointly trained at State key laboratory of Catalysis (SKLC), in Dalian Institute of Chemical Physics (DICP), the Chinese Academy of Sciences. He carried out postdoctoral research in the College of Environment, at Zhejiang University of Technology from 2016 to 2018. Since 2019, he has been working at the Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology. His research interests mainly focus on the development of porous carbon materials and industrial catalysts, mainly include the design, synthesis and catalytic application of carbon-based catalysts, catalytic synthesis of vinyl chloride, green ammonia synthesis and hydrogenation of biomass derived chemicals in aqueous phase. He has coauthored more than 50 peer-reviewed papers.
Ying Li (Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology). Prof. Li Ying received his B.S. degree from Shandong Normal University (P. R. China) in 1998, and Ph.D. degree from Dalian Institute of Chemical Physics, Chinese Academy of Sciences in 2005. She carried out postdoctoral research at Institute of Catalysis, Eindhoven University of Technology (Netherlands) from 2005 to 2007. Since the end of 2007, she has been working in Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology. Her research interests mainly focus on: carbon catalysis, preparation and application of porous carbon, green ammonia synthesis, and carbon-based solid waste resource utilization. She has published more than 200 peer-reviewed papers and 80 patents.
Supported by:
National Key Research and Development Program of China(2024YFC3907904);Joint Fund for Enterprise Innovation Development of the National Natural Science Foundation of China(U23B20162)

摘要/Abstract

摘要：

聚氯乙烯(PVC)由氯乙烯(VCM)通过聚合反应制得, 是我国产能最大的高分子材料之一. 鉴于我国“富煤、贫油、少气”的能源结构现状, 乙炔氢氯化法已成为国内生产氯乙烯单体的主要工艺. 当前, 工业界普遍采用活性炭负载氯化汞催化剂作为氯乙烯生产的催化剂. 然而, 随着全球范围内限汞政策的不断推进, 开发新型的无汞催化剂已成为当务之急. 尽管已有关于金、铜、钌等金属催化剂的研究报道, 但这些催化剂存在金属组分易流失、成本高昂及易因中毒而失活等缺陷. 相比之下, 无金属碳催化剂以其绿色环保、成本低廉且不存在金属烧结与流失问题等优势, 在无汞催化剂领域展现出了巨大的发展潜力. 非金属碳催化剂的开发被视为应对可持续催化挑战的重要途径, 特别是在替代煤基聚氯乙烯工业中有毒且危害环境的汞基催化剂方面, 已引起广泛关注. 自2014年乙炔氢氯化非金属碳催化剂被首次报道以来, 经过了十年的发展, 其催化活性及稳定性都获得了大幅度的提高. 在某些情况下, 非金属碳催化剂甚至表现出优于金属催化剂的性能, 充分展现了其作为汞催化剂可持续替代方案的巨大潜力.

本文系统总结了乙炔氢氯化碳催化剂的最新研究进展, 从碳催化剂的活性位结构认识的发展历程、催化剂的制备方法、催化反应和失活机理, 以及从实验室小试技术迈向大规模工业化应用过程中所面临的诸多挑战等几个方面进行阐述. 首先, 简要介绍了近十年来乙炔氢氯化碳催化剂的研究进展, 特别指出了活性位的识别逐渐深入的过程, 并阐述了不同活性位点(如单掺杂、共掺杂、缺陷、缺陷与杂原子的协同效应及曲率结构)在乙炔氢氯化反应中的作用机制. 然后, 讨论了碳催化剂的合成策略, 包括后处理法和直接碳化法制备杂原子掺杂碳催化剂, 以及高温脱杂原子和刻蚀等技术制备缺陷碳催化剂. 此外, 讨论了乙炔氢氯化碳催化反应机理和失活机理, 以及催化剂稳定和再生策略. 最后, 总结了非金属碳催化剂从实验室研究到工业化过程中可能面临的关键挑战及未来研究方向. 与工业催化剂相比, 非金属碳催化剂的稳定性仍存在较大差距, 亟需加强对催化剂失活机理及积炭物种的分析研究, 探索有效的抑制失活策略. 尽管碳催化剂在实验室规模生产中具有一定优势, 但在工业规模上可能面临成本效益和重复性问题, 因此需开发适用于工业放大生产的非金属碳催化剂. 由于非金属碳催化剂的复杂结构使得其活性位点仍存在争议, 未来应着力开发活性位点明确的非金属碳催化剂. 经济可行性是碳基非金属催化剂能否与金属催化剂竞争的关键, 需优选可持续碳源, 如生物质衍生物和废弃聚合物, 用于制备碳基非金属催化剂. 同时, 考虑到工业原料通常含有杂质, 实验室使用纯试剂的测试结果可能无法反映实际性能, 因此必须验证催化剂在工况条件下的表现.

综上, 本文系统地总结了碳基催化剂在乙炔氢氯化反应中的技术优势、活性位鉴别、合成策略、反应机理以及工业化应用过程中所面临的诸多挑战. 本文不仅为乙炔氢氯化反应中碳基催化剂的实际应用提供了有益的参考, 更为其他多相催化反应中绿色碳催化剂体系的设计与开发提供一定的参考和借鉴.

关键词: 无金属, 碳催化剂, 乙炔氢氯化, 杂原子掺杂, 缺陷工程

Abstract:

The development of metal-free carbon catalysts has garnered significant attention as a promising approach to address the challenges of sustainable catalysis, particularly in the replacement of toxic and environmentally hazardous mercury-based systems for the coal-based PVC industry. Within a decade of development, the catalytic performance of carbon catalysts has been improved greatly and even shows superiorities over metal catalysts in some cases, which have demonstrated great potential as sustainable alternatives to mercury catalysts. This review provides a comprehensive summary of the recent advancements in carbon catalysts for acetylene hydrochlorination. It encompasses a wide range of aspects, including the identification of active sites from heteroatom doping to intrinsic carbon defects, the various synthetic strategies employed, the reaction and deactivation mechanisms of carbon catalysts, and the current insights into the key challenges that are encountered on the journey from laboratory research to scalable commercialization within the field of carbon catalysts. The review offers foundational insights and practical guidelines for designing green carbon catalysts systems, not only for acetylene hydrochlorination but also for other heterogeneous catalytic reactions.

Key words: Metal-free, Carbon catalyst, Acetylene hydrochlorination, Heteroatom doping, Defect engineering

魏抒豪, 蓝国钧, 邱一洋, 林迪, 孔薇, 李瑛. 乙炔氢氯化非金属碳催化剂的研究进展: 从杂原子掺杂到本征缺陷[J]. 催化学报, 2025, 70: 8-43.

Shuhao Wei, Guojun Lan, Yiyang Qiu, Di Lin, Wei Kong, Ying Li. Advances in metal-free carbon catalysts for acetylene hydrochlorination: From heteroatom doping to intrinsic defects over the past decade[J]. Chinese Journal of Catalysis, 2025, 70: 8-43.

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图/表 21

Fig. 1. (a) Metal-free catalysts for acetylene hydrochlorination: From heteroatoms doped carbon to DC. (b) Research history of carbon-based metal-free catalysts (carbon catalysts), space-time yield (STY) of vinyl chloride [5,7,16???????????-28]. Reprinted with permission from Ref. [5,7,16???????????-28]. Copyright 2014, 2017, John Wiley and Sons. Copyright 2014, Springer Nature. Copyright 2014, 2017, 2018, 2019, Elsevier. Copyright 2015, 2017, 2022, American Chemical Society. Copyright 2018, 2019, 2020, Royal Society of Chemistry.

Fig. 2. (a) Overview of active site created on carbons for acetylene hydrochlorination: From heteroatoms doped carbon to carbon defect. (b) The synthetic strategies to carbon catalysts.

Fig. 3. (a) Reaction energy diagram illustrating the key species along the reaction pathway: reactant (Re), co-adsorbed reactants/products (Co-ads), transition state (TS), intermediate product (Im), and product (Pr). (b) The geometries of the substances involved in the reaction path contain the co-adsorbed reactants (Co-ads), transition state (Ts), and intermediate product (Im). Atoms of chlorine, nitrogen, carbon, and hydrogen are represented in green, blue, gray, and white, respectively [16]. Reprinted with permission from Ref. [16]. Copyright 2014, Elsevier. (c) Correlation between acetylene conversion and the -N= content of PoPD polymers [37]. Reprinted with permission from Ref. [37]. Copyright 2021, Royal Society of Chemistry. (d) Acetylene conversion as a function of accessible pyrrolic N sites, estimated by multiplying the pyrrolic N species content by the specific surface area. Reaction conditions: 200 °C, 3.1 mL g-1 min-1, and HCl/C2H2 volume ratio = 1.15: 1. (e) Adsorption structures of acetylene (C2H2) on the catalyst surface. (f) Corresponding adsorption energies (Ea). (g) Projected density of pz states of C sites during C2H2 adsorption [7]. Reprinted with permission from Ref. [7]. Copyright 2014, Springer Nature. (h) Fitting analysis between nitrogen species content and catalytic reactivity. (i) Charge density distribution of the HOMO orbital in NCNT, the LUMO orbital of C2H2, and the bond formation between NCNT and C2H2. Carbon, nitrogen, and hydrogen are depicted in gray, blue, and white, respectively [17]. Reprinted with permission from Ref. [17]. Copyright 2014, John Wiley and Sons.

Fig. 4. (a) Electrostatic potential mapping of the BC3 configuration. (b) Dipole moments of pristine graphene (p-G) and surfaces doped with g-B, BC3, BC2O, and BCO2 species. Inset: Electrostatic potential maps of the corresponding surface models [25]. Reprinted with permission from Ref. [25]. Copyright 2020, Royal Society of Chemistry. (c) Calculated energy profiles of reaction pathways for the five distinct active sites. (d) Configurations of B or N dopants in single-walled carbon nanotube (SWCNTs), including pyridine around a vacancy (1), pyridine at the zigzag edge (7), pyridine at the armchair edge (9), pyrrolic (5), and graphitic (3); (e) Adsorption energies of C2H2 on various dopant configurations; (c) Bader charge analysis for C2H2 adsorbed on doped SWCNTs [53]. Reprinted with permission from Ref. [53]. Copyright 2019, Elsevier.

Fig. 5. On-site Bader charge (a) and spin density isosurface (c) for the undoped model carbon layer. On-site Bader charge (b) and spin density isosurface (d) for the doped model carbon layer, providing insights into the catalytic mechanism. C2H2-TPD (e) and HCl-TPD (f) profiles. (g) Charge density difference and the corresponding plane-averaged charge density difference along the z-direction for S-QDs. (h) Projected density of states (PDOS) of S p orbitals in S-QDs and the molecular orbital of C2H2, with an inset showing the charge density difference between C2H2 and S-QDs (isosurface: 0.04 au). (i,j) Reaction pathways for acetylene hydrochlorination over S-QDs [40]. Reprinted with permission from Ref. [40]. Copyright 2024, American Chemical Society.

Fig. 6. (a) Adsorption energy (Eads) of HCl on various active sites in N-G and B, N-G catalysts: (I) carbon atoms bonded to pyridinic N species, (II) carbon atoms bonded to pyrrolic N species, and (III) carbon atoms bonded to graphitic N species. (b) TPD profiles of GO, N-G, and B, N-G [18]. Reprinted with permission from Ref. [18]. Copyright 2015, American Chemical Society. Charge density difference contour plots obtained via DFT calculations for pyridinic N (c), pyridinic N (d) adjacent to sulfide groups, pyrrolic N (e), and pyrrolic N (f) adjacent to sulfide groups, with corresponding Bader charges for relevant C and N atoms shown in red [20]. (g) Possible catalyst structures with adsorbed C2H2: pyrrolic N (structure 1), quaternary N (structure 2), pyridinic N (structure 3), pyridinic N+O? (structure 4), P-C (structure 5), para-position NP (structure 6), and ortho-position NP (structure 7). (h) Adsorption energies (E?) of C2H2 on these structures. (i) Calculated energy profiles of the reaction pathways using para-position (structure 6) and ortho-position (structure 7) as active sites. Blue, gray, white, and pink spheres represent N, C, H, and P atoms, respectively [39]. Reprinted with permission from Ref. [39]. Copyright 2019, Elsevier.

Fig. 7. TEM images of nanodiamond (ND) (a) and ND@G (b). (c) Raman spectra of various carbon materials. (d) Acetylene conversion over various catalysts during acetylene hydrochlorination. Reaction conditions: 220 °C, gas hourly space velocity (GHSV) of C2H2 = 300 h-1. (e) The stability test of ND@G in acetylene hydrochlorination (220 °C, GHSV of C2H2 = 30 h-1) [23]. Reprinted with permission from Ref. [23]. Copyright 2019, Royal Society of Chemistry.

Fig. 8. (a) The relationship of catalytic activity of defective AC with ID/IG calculated by Raman spectra. (b) Reaction pathways along zigzag (green) and armchair (blue) edges of graphene [24]. Reprinted with permission from Ref. [24]. Copyright 2019, Elsevier. Correlation between the reaction rate and (c) sp3% in sp2-oriented carbon catalysts, and (d) sp2% in sp3-oriented carbon catalysts. (e) Reaction pathways of carbon materials with varying sp2:sp3 ratios were calculated using DFT. (f) Charge density differences of C2H2 adsorption on the diamond (111) surface with sp2:sp3 = 0.08 and sp2:sp3 = 0.75. Blue regions represent holes, while yellow regions indicate electrons. The charges on the two carbon atoms in acetylene are also annotated [27]. Reprinted with permission from Ref. [27]. Copyright 2020, Royal Society of Chemistry.

Fig. 9. (a) Raman spectra of catalysts. (b) Acetylene conversion over C700, C900, and C1100 catalysts under reaction conditions of 220 °C and a GHSV of C2H2 = 36 h-1. TPD evolution profiles for C2H2 (c) and HCl (d) on the catalysts. The most stable adsorption structures of HCl (e) and C2H2 (f) [22]. Reprinted with permission from Ref. [22]. Copyright 2018, Elsevier. (g) Optimized adsorption geometries of acetylene and HCl on P-g-C3N4 and F-g-C3N4, along with the corresponding adsorption energies. Blue, gray, white, and green spheres represent nitrogen, carbon, hydrogen, and chlorine atoms, respectively. Bond lengths are provided in ?. (h) Reaction energy diagrams for acetylene hydrochlorination on F-g-C3N4-N1 and P-g-C3N4 [91]. Reprinted with permission from Ref. [91]. Copyright 2019, Royal Society of Chemistry.

Fig. 10. Theoretical investigations. The adsorbed energies of C2H2 (a) and HCl (b) on the plane, out-curved and in-curved surfaces. When the adsorbates are located on the outer side of the curved surface, the surface is called the outward curved surface (out-curved surface) in this work. When the adsorbates are on the inner side of the curved surface, the surface is referred to as the inward curved surface (in-curved surface). (c) The reaction pathways of acetylene hydrochlorination on the surfaces. Reaction states A, B, C, D, and E are described in the main text. Blue, white, and grey balls indicate the N, H, and C atoms, respectively. Reaction pathway of acetylene hydrochlorination on N doped. (d) The TEM of HCDC. (e) Conversion of acetylene in the acetylene hydrochlorination reaction. Reaction conditions: 220 °C, GHSV(C2H2) = 300 h-1, and V(HCl):V(C2H2) = 1.2: 1. (f) The adsorption of C2H2 adsorbed in the per specific surface area of catalysts. (g) Reaction orders of HCl and (h) C2H2 for HCDC and DC. Reaction conditions: catalyst (0.1 g), 220 °C, and ambient pressure. The concentrations of C2H2 and HCl from 10% to 25% balanced in N2 flow. The reaction order of both reactants is indicated by the slope of the fitting lines. (i) Adsorption diagram of C2H2 and HCl molecules on the surfaces of different catalysts [92].

Table 1 The key information of various carbon catalysts in acetylene hydrochlorination.

Catalysts	Active site	Carbon precursor	Temperature (°C)	GHSV (h^-1)	Conv. (%)	STY g_vcm g_cat^-1 h^-1	Ref.
B, N-MC(0.5)	B-N	polymer	220	300	62	0.87	[57]
S-QDs	S-S	quantum do	180	50	66		[40]
CN-800	pyridinic N	ionic liquid	220	360	74	1.38	[97]
0.3PmPD-C-800	N content	polymer	220	150	96.4	0.14	[98]
CTN-700	pyridinic N	polymer	220	40	99.3		[99]
D-GC-800	pyridinic N	biomass	180	36	96		[100]
NPCs-T	pyridine N; pyridinic N⁺O; defects	polymer	180	30	90.9		[101]
Chi800	pyridinic N; pyrrolic N	polymer	220	36	91		[102]
2.5DF/BC-850	quaternary N	biomass	220	45	94.5		[103]
1.00NPC	pyridinic N; pyrrolic N; defects	polymer	220	300	30	1.72	[26]
ACF	defect	AC	180	30	80		[104]
ND-900	defect	ND	220	50	90.6	0.14	[105]
MPF-800	pyridinic N; defects	polymer	180	30	86		[106]
PACP-800	pyridinic N⁺O^-	polymer	180	30	84		[28]
20%[DBU][Cl]/AC	[DBU][Cl]	ionic liquid	240	30	86.7		[107]
U-NC-550	pyrrolic N	polymer	260	200	75.86	1.6	[56]
NC4P (0.5)-0.5	pyridinic N	polymer	260	30	88	0.16	[58]
NC	pyrrolic N	polymer	140	30	47		[108]
PoPD-70-300	pyridinic N	polymer	280	30	95	0.16	[37]
NC-800	pyridinic N; pyrrolic N; defects	polymer	220	30	98		[45]
N@CBC-FE	nitrogen defects	polymer	220	180	60		[109]
N-CB-800	nitrogen defects	waste	220	100	71.8	0.35	[110]
1H-imidazole	pyrrolic N	imidazole	220	30	60		[111]
B-CNDs	BC₃	ponic liquid	220	500	58	1.19	[25]
SBMC-800	pyrrolic N	biomass	200	110	99	0.17	[112]
ND-1100	defect	ND	220	300	83	0.69	[27]
3% S/B-SAC	C-S bond	AC	180	90	45		[72]
NC-800-700	pyridinic N	polymer	260	30	98.7	0.37	[44]
CN-2	pyrrolic N	polymer	220	50	98.1		[113]
CBC	defects	AC	180	36	33		[114]
HMT/AC	quaternary N	AC	220	30	60		[115]
NP-C600	NP-C	ionic liquid	220	30	99.2	1.15	[39]
D-AC-M	defect	AC	220	30	61.6	0.15	[24]
MF-600	nitrogen defects	polymer	220	30	90	0.35	[91]
PAN-400-air-N₂	pyridinic N	polymer	280	50	93	0.16	[62]
3NR/4CAC	nitrogen	AC	220	30	97.9	0.36	[38]
ND@G-900	defects	ND	220	30	85.5	0.12	[23]
[Bmim]Cl		ionic liquids	180	40	35		[116]
S, N-Carbon-2.5	pyrrolic N	polymer	180	50	82.4	0.19	[49]
C1100	defects	polymer	220	36	95.4	0.38	[22]
NPC-800	the nitrogen	polymer	220	30	98	0.28	[117]
17% ZIF-8/SAC	the nitrogen	AC	220	30	81	0.62	[36]
N-MC-G	quaternary N	biomass	220	30	85.5	0.2	[21]
NS-C-NH₃	pyridinic N	biomass	220	26	80	0.70	[20]
h-BN	defects	BN	280	44	99	0.21	[19]
AC-n-U500	pyrrolic N; quaternary N	AC	210	50	92	0.46	[118]
Z₄M₁	pyridinic N	MOF	180	50	60	0.15	[96]
N-OMC-2.0	quaternary N	biomass	180	50	35	0.09	[119]
PANI-AC	pyrrolic N	AC	180	36	76.3	0.20	[59]
B, N-G	pyridinic N	graphene	250	36	94.9	0.29	[18]
g-C₃N₄/AC	the nitrogen	AC	180	50	76.5	0.32	[16]
SiC@N-C	pyrrolic N	polymer	200	30	80	0.11	[7]
N-CNTs	quaternary N	CNT	180	180	10	0.17	[17]

Table 1 The key information of various carbon catalysts in acetylene hydrochlorination.

Catalysts	Active site	Carbon precursor	Temperature (°C)	GHSV (h^-1)	Conv. (%)	STY g_vcm g_cat^-1 h^-1	Ref.
B, N-MC(0.5)	B-N	polymer	220	300	62	0.87	[57]
S-QDs	S-S	quantum do	180	50	66		[40]
CN-800	pyridinic N	ionic liquid	220	360	74	1.38	[97]
0.3PmPD-C-800	N content	polymer	220	150	96.4	0.14	[98]
CTN-700	pyridinic N	polymer	220	40	99.3		[99]
D-GC-800	pyridinic N	biomass	180	36	96		[100]
NPCs-T	pyridine N; pyridinic N⁺O; defects	polymer	180	30	90.9		[101]
Chi800	pyridinic N; pyrrolic N	polymer	220	36	91		[102]
2.5DF/BC-850	quaternary N	biomass	220	45	94.5		[103]
1.00NPC	pyridinic N; pyrrolic N; defects	polymer	220	300	30	1.72	[26]
ACF	defect	AC	180	30	80		[104]
ND-900	defect	ND	220	50	90.6	0.14	[105]
MPF-800	pyridinic N; defects	polymer	180	30	86		[106]
PACP-800	pyridinic N⁺O^-	polymer	180	30	84		[28]
20%[DBU][Cl]/AC	[DBU][Cl]	ionic liquid	240	30	86.7		[107]
U-NC-550	pyrrolic N	polymer	260	200	75.86	1.6	[56]
NC4P (0.5)-0.5	pyridinic N	polymer	260	30	88	0.16	[58]
NC	pyrrolic N	polymer	140	30	47		[108]
PoPD-70-300	pyridinic N	polymer	280	30	95	0.16	[37]
NC-800	pyridinic N; pyrrolic N; defects	polymer	220	30	98		[45]
N@CBC-FE	nitrogen defects	polymer	220	180	60		[109]
N-CB-800	nitrogen defects	waste	220	100	71.8	0.35	[110]
1H-imidazole	pyrrolic N	imidazole	220	30	60		[111]
B-CNDs	BC₃	ponic liquid	220	500	58	1.19	[25]
SBMC-800	pyrrolic N	biomass	200	110	99	0.17	[112]
ND-1100	defect	ND	220	300	83	0.69	[27]
3% S/B-SAC	C-S bond	AC	180	90	45		[72]
NC-800-700	pyridinic N	polymer	260	30	98.7	0.37	[44]
CN-2	pyrrolic N	polymer	220	50	98.1		[113]
CBC	defects	AC	180	36	33		[114]
HMT/AC	quaternary N	AC	220	30	60		[115]
NP-C600	NP-C	ionic liquid	220	30	99.2	1.15	[39]
D-AC-M	defect	AC	220	30	61.6	0.15	[24]
MF-600	nitrogen defects	polymer	220	30	90	0.35	[91]
PAN-400-air-N₂	pyridinic N	polymer	280	50	93	0.16	[62]
3NR/4CAC	nitrogen	AC	220	30	97.9	0.36	[38]
ND@G-900	defects	ND	220	30	85.5	0.12	[23]
[Bmim]Cl		ionic liquids	180	40	35		[116]
S, N-Carbon-2.5	pyrrolic N	polymer	180	50	82.4	0.19	[49]
C1100	defects	polymer	220	36	95.4	0.38	[22]
NPC-800	the nitrogen	polymer	220	30	98	0.28	[117]
17% ZIF-8/SAC	the nitrogen	AC	220	30	81	0.62	[36]
N-MC-G	quaternary N	biomass	220	30	85.5	0.2	[21]
NS-C-NH₃	pyridinic N	biomass	220	26	80	0.70	[20]
h-BN	defects	BN	280	44	99	0.21	[19]
AC-n-U500	pyrrolic N; quaternary N	AC	210	50	92	0.46	[118]
Z₄M₁	pyridinic N	MOF	180	50	60	0.15	[96]
N-OMC-2.0	quaternary N	biomass	180	50	35	0.09	[119]
PANI-AC	pyrrolic N	AC	180	36	76.3	0.20	[59]
B, N-G	pyridinic N	graphene	250	36	94.9	0.29	[18]
g-C₃N₄/AC	the nitrogen	AC	180	50	76.5	0.32	[16]
SiC@N-C	pyrrolic N	polymer	200	30	80	0.11	[7]
N-CNTs	quaternary N	CNT	180	180	10	0.17	[17]

Fig. 11. (a) Schematic for synthesis of SiC@N-C nanocomposite. (b) high-resolution transmission electron microscopy (HRTEM) image of SiC@N-C showing a core-shell-like morphology (scale bar, 2 nm). (c) XPS N1s spectrum for the SiC@N-C catalyst with a total N content of 7.1% [7]. Reprinted with permission from Ref. [7]. Copyright 2014, Springer Nature. (d) The preparation process of N-doped AC. (e) The simulated process of amino N doping into AC to form pyridine nitrogen [38]. Reprinted with permission from Ref. [38]. Copyright 2019, Elsevier.

Fig. 12. (a) The synthesis of NP-C600. (b) The calculated STY (gvcm hcat-1 g-1) values of NPC600 and other catalyst materials [39]. Reprinted with permission from Ref. [39]. Copyright 2019, Elsevier. The dual-[pyrrolic + pyridinic N] site (c) and the dual-[pyrrolic + pyridinic N] site (d), the pyridinic N was strongly adsorbed by HCl in this dual N site. The blue, red, grey, green, black, and white balls represent the N atom in pyrrolic N, the N atom in pyridinic N, the C atom in the carrier, the Cl atom, the C atom in C2H2 and the H atom, respectively [130]. Reprinted with permission from Ref. [130]. Copyright 2020, Royal Society of Chemistry. Conversion of acetylene over B-CNDs at different reaction temperatures and GHSV (e), at total GHSVs of 1000 h-1 and reaction temperature of 220 °C (f). Insertion: TEM image of used B-CNDs. (g) Specific B content estimated from XPS. (h) The calculated STY values of various metal-free catalysts [25]. Reprinted with permission from Ref. [25]. Copyright 2020, Royal Society of Chemistry.

Fig. 13. (a) The preparation process of nitrogen-doped mesoporous carbon (N-MC-W) using wheat flour as both carbon and nitrogen sources. (b) Stability test of N-MC-GAC and MCN in acetylene hydrochlorination under reaction conditions of 220 °C, 0.1 MPa, and GHSV = 30 h-1. (c) N 1s XPS spectra of N-MC-G and MCN, showing the nitrogen configurations [21]. Reprinted with permission from Ref. [21]. Copyright 2018, Royal Society of Chemistry. (d) Schematic illustration of the synthesis process for N-doped biochar derived from walnut shells. SEM images of 2.5DF/BC-850, highlighting its morphology (e) and SEM images of 2.5DF/BC-850 after use, showing its structural stability (f) [103]. Reprinted with permission from Ref. [103]. Copyright 2022, Elsevier.

Fig. 14. (a) Schematic illustration of the synthesis of ZIF-8/SAC composite. (b) TEM images of nanoparticles in 17% ZIF-8/SAC catalyst. (c) The corresponding particle size histograms of the nanoparticles [36]. Reprinted with permission from Ref. [36]. Copyright 2017, Springer Nature.

Fig. 15. (a) Schematic diagram illustrating the synthesis process of PAN-derived materials. (b) High-resolution XPS N 1s spectra of PAN and PAN-derived materials, showing the suggested structures of all nitrogen species. (c) Illustration of three proposed models used in DFT calculations [62]. Reprinted with permission from Ref. [62]. Copyright 2019, American Chemical Society. (d) Schematic representation of N-doped carbon catalyst synthesis via traditional and sonochemistry methods. SEM image of UAPFS (e) and U-NC-550 (f). TEM image (g) and TEM mapping images (h) of U-NC-550 catalysts, highlighting the distribution of dopants. (i) FT-IR spectra comparing U-APFS and T-APFS. (j) EPR spectra of T-APFS and U-APFS carbon precursors. (k) Raman spectra of the synthesized catalysts [56]. Reprinted with permission from Ref. [56]. Copyright 2022, Springer Nature.

Fig. 16. (a) Resource utilization of PVC plastics. N 1s XPS spectra (b) and Raman spectra (c) of various of various xNPC prepared with different mass ratios of melamine and PVC (x = 0.25, 0.50, 0.75, 1.00, 2.00) [26]. Reprinted with permission from Ref. [26]. Copyright 2022, American Chemical Society. (d) Synthetic steps involved in the preparation of NCs with varying textural properties at a fixed N-content and speciation. (e) Ar adsorption (filled) and desorption (open) isotherms of NC-I, NC-II, NC-III and their pore size distribution calculated via NLDFT method. (f) Time-on-stream (TOS) performance of the NC series is indicated as the normalized yield of vinyl chloride monomer (Y(VCM)) [148]. Reprinted with permission from Ref. [148]. Copyright 2020, John Wiley and Sons.

Fig. 17. (a) The schematic of the formation of Defect Graphene [83]. Reprinted with permission from Ref. [83]. Copyright 2016, John Wiley and Sons. (b) Schematic illustration for the synthesis of NC. (c) Peak area spectrum fitting for Raman spectra of catalysts. (d) Relationship between nitrogen content, carbon defects, and acetylene conversion [45]. Reprinted with permission from Ref. [45]. Copyright 2020, Elsevier. (e) The preparation process of the defect-rich carbon materials. (f) The relationship of catalytic activity of defective AC with ID/IG was calculated by Raman spectra [24]. Reprinted with permission from Ref. [24]. Copyright 2019, Elsevier.

Fig. 18. (a) Schematic of preparing the D-HOPG sample. (b) SEM image of D-HOPG. N 1s XPS spectra (c) and Raman spectra (d) of HOPG (purple), Ar-HOPG (blue), N-HOPG (red), and D-HOPG (black). (e,f) Preparation and structural characterization of high-defect density porous carbon [80]. Reprinted with permission from Ref. [80]. Copyright 2019, Springer Nature. (e) Design and fabrication schematic diagram of high-defect density porous carbon (HDPC). (g) TEM image of ZnO@ZIF-7. (h) HRTEM image of a representative ZnO QD encapsulated by ZIF-7. (i) High-resolution transmission electron microscopy (HRTEM) of HDPC. (j) Magnification of one segment of the HRTEM after fast Fourier transformation (FFT) filtering. (k) EPR spectrum of LDPC and HDPC [82]. Reprinted with permission from Ref. [82]. Copyright 2020, Elsevier.

Fig. 19. (a,b) The reaction pathways of acetylene hydrochlorination on the surfaces are followed by the Eley-Rideal (ER) mechanism. (c) The reaction pathways of acetylene hydrochlorination on the surfaces are followed by the Langmuir-Hinshelwood (LH) mechanism. (d) Long-term evaluations of NC600, NC700, and NC900 catalysts. Reaction conditions: 180 °C, GHSV = 90 h-1, V(HCl)/V(C2H2) = 1.2 and P = 1 bar. The optimized structures along the pathway are shown at the bottom [130]. Reprinted with permission from Ref. [130]. Copyright 2020, Royal Society of Chemistry. (e) Optimized structure of C2H2 adsorption and HCl adsorption on pristine, mono- and divacancy, Stone Wales defect, armchair edge, and zigzag edge defected SWCNTs. The gray, white, green, and magenta colors represent carbon atoms in SWCNT, hydrogen atoms, chlorine atoms, and carbon atoms in acetylene molecules, respectively. (f) The reaction pathway of acetylene hydrochlorination. TS1 and TS2 signify the transition states. The zero points for energy represent the reactants (HCl and C2H2) in the gas phase and defected SWCNT. The adsorption energy and the barrier are measured in eV. The structures A, B, C, D, and F on these reaction pathways are also included [155]. Reprinted with permission from Ref. [155]. Copyright 2020, John Wiley and Sons.

Fig. 20. (a) The acetylene conversion over time of catalysts with different boron additions and modifications at 30 h-1, reaction conditions: 220 °C, and the volume ratio of hydrogen chloride to acetylene is 1.2:1. (b) Ar-TPD-MS of used catalysts, m/e = 78. C2H2-TPSR of D-NMCS (c) and D-BNMCS-0.5 (d). The polymerization reaction paths of acetylene on different models: N-doped model (e), B, N co-doped model (f) [57]. Reprinted with permission from Ref. [57]. Copyright 2024, Elsevier. (g) Stability test of PDA/SiC-700 for a 1000-h and its catalytic activity upon regeneration by high-temperature NH3-treatment. Reaction conditions: 200 °C and space velocity 0.8 ml g?1 min?1. (h) Effluents during regeneration of PDA/SiC-700-p monitored by an online MS (a) in 6% NH3 (He balanced); with m/e = 27 (pink curve) corresponding to HCN and C2H3Cl; with m/e = 62 (green curve) corresponding to C2H3Cl; m/e = 18 (blue curve) corresponding to H2O; and m/e = 17 (red curve) corresponding to NH3. (For interpretation of the references to color in this Fig. legend, the reader is referred to the web version of this article) [5]. Reprinted with permission from Ref. [5]. Copyright 2017, Elsevier. (i) Stability test of D-GH-800 and 0.5ZnCl2/Used-800. Reaction conditions: T = 180 °C, C2H2 = 180 h-1, VHCl/VC2H2 = 1.15.

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乙炔氢氯化非金属碳催化剂的研究进展: 从杂原子掺杂到本征缺陷

Advances in metal-free carbon catalysts for acetylene hydrochlorination: From heteroatom doping to intrinsic defects over the past decade

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