Insights into carbon-based materials for catalytic dehydrogenation of low-carbon alkanes and ethylbenzene

doi:10.1007/s11705-023-2328-6

Front. Chem. Sci. Eng.

2023, Vol. 17

Issue (11) : 1623-1648 https://doi.org/10.1007/s11705-023-2328-6

REVIEW ARTICLE

Insights into carbon-based materials for catalytic dehydrogenation of low-carbon alkanes and ethylbenzene

Sijia Xing¹, Sixiang Zhai¹, Lei Chen¹, Huabin Yang^1,², Zhong-Yong Yuan^1,²(

)

¹. School of Materials Science and Engineering, Smart Sensing Interdisciplinary Science Center, Nankai University, Tianjin 300350, China
². Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), Nankai University, Tianjin 300071, China

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Abstract

Direct dehydrogenation with high selectivity and oxidative dehydrogenation with low thermal limit has been regarded as promising methods to solve the increasing demands of light olefins and styrene. Metal-based catalysts have shown remarkable performance for these reactions, such as Pt, CrO_x, Co, ZrO_x, Zn and V. Compared with metal-based catalysts, carbon materials with stable structure, rich pore texture and large surface area, are ideal platforms as the catalysts and the supports for dehydrogenation reactions. In this review, carbon materials applied in direct dehydrogenation and oxidative dehydrogenation reactions including ordered mesoporous carbon, carbon nanodiamond, carbon nanotubes, graphene and activated carbon, are summarized. A general introduction to the dehydrogenation mechanism and active sites of carbon catalysts is briefly presented to provide a deep understanding of the carbon-based materials used in dehydrogenation reactions. The unique structure of each carbon material is presented, and the diversified synthesis methods of carbon catalysts are clarified. The approaches for promoting the catalytic activity of carbon catalysts are elaborated with respect to preparation method optimization, suitable structure design and heteroatom doping. The regeneration mechanism of carbon-based catalysts is discussed for providing guidance on catalytic performance enhancement. In addition, carbon materials as the support of metal-based catalysts contribute to exploiting the excellent catalytic performance of catalysts due to superior structural characteristics. In the end, the challenges in current research and strategies for future improvements are proposed.

Keywords carbon materials dehydrogenation active sites mechanism catalytic performance support

Corresponding Author(s): Zhong-Yong Yuan

About author:

Peng Lei and Charity Ngina Mwangi contributed equally to this work.

Just Accepted Date: 22 May 2023 Online First Date: 03 July 2023 Issue Date: 25 October 2023

Cite this article:

Sijia Xing,Sixiang Zhai,Lei Chen, et al. Insights into carbon-based materials for catalytic dehydrogenation of low-carbon alkanes and ethylbenzene[J]. Front. Chem. Sci. Eng., 2023, 17(11): 1623-1648.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-023-2328-6
https://academic.hep.com.cn/fcse/EN/Y2023/V17/I11/1623

Tab.1 Different features of DH and ODH of low-carbon alkane

Fig.1 Schematic illustration of active sites and mechanisms of carbon catalysts in DH and ODH reactions (ordered mesoporous carbon, OMC).

Fig.2 (a) N₂ adsorption-desorption isotherms of MCs; (b) TEM images of MC-2-600 catalysts; (c) propane conversion and propylene selectivity of MCs as a function of carbonization temperature; (d) the specific activity of MC-2-y catalysts as a function of carbonization temperature (y represents carbonization temperature of 600, 700 and 800 °C). Reprinted with permission from Ref. [69], copyright 2019, Elsevier.

Fig.3 Active sites identification: C=O. (a) TPD-MS (mass sepetrometry) curves of oxidized MWCNTs and (b) thermally treated so-MWCNTs. (c) O 1s XPS spectra of raw oxidized MWCNTs. Initial propylene formation rates of oxidized MWCNTs as functions of a number of carbonyl groups, calculated from (d) XPS analysis and (e) TPD-MS results. (f) Schematic illustration of the PDH process on MWCNTs. Reprinted with permission from Ref. [60], copyright 2018, Elsevier.

Fig.4 Catalytic performance enhancement: (a) preparation method optimization of oxidative CNTs through solid–solid treatment. Reprinted with permission from Ref. [81], copyright 2017, Wiley-VCH. (b) Heteroatoms doping by Grignard reduction on o-CNT in ODH of n-butane. Reprinted with permission from Ref. [82], copyright 2018, Elsevier.

Fig.5 (a) Fourier-filtered image of high-resolution TEM (HRTEM) image of the ND/FLG catalyst shows the pure diamond lattices with the elimination of graphene lattices; (b) schematic model illustrating the NDs anchored on the surface of graphene; (c, d) catalytic performance of carbon catalysts. Reprinted with permission from Ref. [96], copyright 2015, Elsevier.

Fig.6 Typical HRTEM images of (a) pristine ND, (b) ND-800, (c) ND-1000 and (d) ND-1300 (ND-x, x = annealing temperature); (e) catalytic performance of nanocarbon samples after 8 h on stream. Reprinted with permissiom from Ref. [55], copyright 2014, Wiley-VCH.

Fig.7 Structure characterization: (a) HRTEM images and (b) corresponding magnification images of AC-based catalysts. Catalytic performance: (c) DH selectivity of AC-based catalysts and (d) long-term stability test of 1500AC catalyst at 400 °C. Reprinted with permission from Ref. [136], copyright 2021, Elsevier.

Fig.8 (a) Schematic illustration of the formation and (b) catalytic performance of the PDA hollow nanosphere carbon-based catalysts (TEOS: tetraethyl orthosilicate; TOF: turnover frequency). Reprinted with permission from Ref. [143], copyright 2021, Elsevier.

Carbon material	Catalyst	Method	S_BET /(m²·g^–1)	Flow rate /(mL·min^–1)	Feed composition	Reaction temperature /°C	Reactant/target product	Conversion^a) /%	Steady-state rate^b)/(mmol·g^–1·h^–1)	Selectivity^c)/%	Catalyst life^d)/h	Ref.
OMC	OMC-1	DH	624	40	C₃H₈/N₂ = 1:19	600	Propane/propylene	69.3–44.5	–	62.2–85.1	100	[68]
	OMC-2	DH	610	40	C₃H₈/N₂ = 1:19	600	Propane/propylene	65.7–39.3	–	70.6–88.6	100	[68]
	MC-2-600	DH	604	40	C₃H₈/N₂ = 1:19	600	Propane/propylene	35.7–28.1	–	85.6–89.4	10	[69]
	HOMC	DH	675	40	C₃H₈/N₂ = 1:19	600	Propane/propylene	20.1–10.3	–	66.1–78.5	50	[70]
	COMC	DH	758	40	C₃H₈/N₂ = 1:19	600	Propane/propylene	22.6–12.1	–	89.0–95.1	50	[70]
	MC	DH	598	40	C₃H₈/N₂ = 1:19	600	Propane/propylene	19.6–9.78	–	87.1–92.6	50	[71]
	MCO	DH	310	40	C₃H₈/N₂ = 1:19	600	Propane/propylene	32.9–21.2	–	66.3–86.6	50	[71]
	CN-15-2.0	ODH	672	20	C₃H₈/O₂/N₂ = 1:1:8	450	Propane/propylene	22.98	–	41.7	\	[72]
	SK	ODH	1205	50	C₈H₁₀/O₂/He = 1:1:124	350	EB/ST	34.0–14.1	–	96.1–96.0	6	[73]
	SK-N	ODH	1415	50	C₈H₁₀/O₂/He = 1:1:124	350	EB/ST	38.7–19.2	–	96.3–96.6	6	[73]
	PMC	DH	679	20	C₃H₈/N₂ = 1:19	600	Propane/propylene	37.1	–	89.2	24	[75]
	BMC	DH	690	20	C₃H₈/N₂ = 1:19	600	Propane/propylene	33.9	–	87.2	24	[75]
	NMC	DH	908	20	C₃H₈/N₂ = 1:19	600	Propane/propylene	18.6	–	84.6	24	[75]
	MC	DH	736	20	C₃H₈/N₂ = 1:20	600	Propane/propylene	30.9	–	87.6	24	[75]
CNTs	CNT-R	ODH	184	10	C₈H₁₀/O₂ = 1:5	400	EB/ST	45	–	86	12	[78]
	MWCNT	DH	150	10	C₂H₆/Ar = 1:1	700	Ethane/ethylene	20–18	–	83–90	75	[60]
	so-MWCNTs	DH	134	20	C₃H₈/N₂ = 1:19	600	Propane/propylene	11.2–5.8	–	92.1–87.9	4	[60]
	5B-oCNTs	ODH	262	15	C₃H₈/O₂/N₂ = 1:1:48	400	Propane/propylene	30	–	70	200	[84]
	PZS@OCNT-800	ODH	306	15	C₃H₈/O₂/He = 1:0.5:48	520	Propane/propylene	14.3	–	63	20	[89]
ND	ND/FLG	DH	134	30	C₈H₁₀/He = 1:35	600	EB/ST	–	19.23	95	–	[96]
	HD-ND/G	DH	–	10	C₈H₁₀/He = 1:37	550	EB/ST	–	36.5–34.2	~97.5–97	60	[97]
	FLG-GO@NDs	DH	304	30	C₃H₈/N₂ = 1:35	550	EB/ST	35.1	–	98.6	50	[98]
	ND-CNT-SDS/SiC	DH	–	10	C₈H₁₀/He = 1:36	550	EB/ST	–	6.25	99.5	20	[101]
	ND-1100	DH	350	15	C₃H₈/N₂ = 1:49	550	Propane/propylene	10.6	–	90	8	[55]
	ND@NMC-700	DH	305	30	C₈H₁₀/Ar = 1:35	700	EB/ST	37.7	5.8	99.6	20	[106]
	N,O-ND/CNT-d	DH	303	10	C₈H₁₀/Ar = 1:35	550	EB/ST	–	5.2	98.7	\	[107]
	ND/CNT-SiC-ms-HN	DH	–	10	C₈H₁₀/Ar = 1:35	550	EB/ST	–	5.49	98.4	20	[108]
	ND/CN-ms-o	DH	702	10	C₈H₁₀/Ar = 1:35	550	EB/ST	–	7.06	~100	20	[109]
	F-ND	ODH	275	10	C₈H₁₀/O₂/N₂ = 1:3:	400	EB/ST	70.8–~50	–	~90	500	[110]
Graphene	rGO	DH	90	10	C₂H₆/Ar = 1:1	700	Ethane/ethylene	~13		90	75	[78]
Graphene	RGO	DH	48	–	C₂H₆/Ar = 1:2	450	Ethane/ethylene	16.5	–	95%	450	[114]
AC	BDAC-700	DH	1078	20	C₃H₈/N₂ = 1:19	600	Propane/propylene	54.2–29.7	–	85.8–91.4	50	[130]
	MC-700	DH	849.2	20	C₃H₈/Ar = 1:19	600	Propane/propylene	36–28	–	70–75	8	[131]
	CMSC-3-700	DH	1400	20	C₃H₈/N₂ = 1:19	600	Propane/propylene	24.7	–	93.5	10	[132]
	CSAC	DH	1190	20	C₄H₁₀/N₂ = 1:19	625	Isobutane/isobutene	71–34	–	~76	72	[57]
	SCW-650	ODH	1438	30	C₄H₁₀/O₂/N₂ = 1:0.5:6	375	Isobutane/isobutene	~9	–	~93	5	[133]
	HC-N-B	ODH	993	40	C₃H₈/CO₂/Ar = 1:2:37	350	Propane/propylene	9–7.8	–	~93	5	[137]
Others	CNFs	ODH	61.5	10	C₈H₁₀/O₂ = 1:5	400	EB/ST	30–25	–	80–75	168	[138]
	B_0.1CN	ODH	181	–	C₂H₆/O₂/N₂ = 1:0.5:23.5	450	Ethane/ethylene	8	–	55	7	[140]
	ND/CNF-FLG	DH	209	30	C₈H₁₀/He = 1:35	600	EB/ST	54–53.5	–	87–85.9	20	[141]
	CF/CNF	DH	259	30	C₈H₁₀/He = 1:35	550	EB/ST	21.9	–	97	25	[142]
	PDA HNSs	ODH	641.6	12.23	C₈H₁₀/O₂/He = 1:0.5:98.5	700	EB/ST	61.6	–	90	16	[143]
	SiC@C	DH	410.3	10	C₈H₁₀/He = 1:35	550	EB/ST	–	11.58	96.86	15	[144]
	C-2	ODH	1318	50	C₈H₁₀/O₂/He = 1:1:124	300	EB/ST	29.1–18.4	–	91.5–91.2	6	[145]

Tab.2 Summary of the catalytic data of carbon materials as the catalysts for DH and ODH reaction

Tab.3 Summary of the catalytic data of carbon materials as the supports of metal-based catalysts for DH and ODH reaction

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