Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO<sub>2</sub> catalysts

HUANG Lizhi; LIU Yali; WEI Qinhong; WANG Luhui

doi:10.12434/j.issn.2097-2547.20250005

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Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO₂ catalysts

更新时间：2025-10-22

- Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO₂ catalysts
- Vol. 50, Issue 10, Pages: 19-26(2025)
- 作者机构：
  
  1.浙江海洋大学全省临港石化污染控制重点实验室，浙江舟山 316022
  2.浙江海洋大学临港石油天然气储运技术国家地方联合工程研究中心，浙江舟山 316022
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20250005
  CLC： TQ426
- Received：05 January 2025，
  
  Revised：2025-01-25，
  
  Published：25 October 2025
- 稿件说明：
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黄礼智,刘亚丽,魏勤洪等.三维介孔Ni-ZrO₂催化剂甲烷干重整性能研究[J].低碳化学与化工,2025,50(10):19-26.

HUANG Lizhi,LIU Yali,WEI Qinhong,et al.Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO₂ catalysts[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(10):19-26.
黄礼智,刘亚丽,魏勤洪等.三维介孔Ni-ZrO₂催化剂甲烷干重整性能研究[J].低碳化学与化工,2025,50(10):19-26. DOI： 10.12434/j.issn.2097-2547.20250005.

HUANG Lizhi,LIU Yali,WEI Qinhong,et al.Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO₂ catalysts[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(10):19-26. DOI： 10.12434/j.issn.2097-2547.20250005.

摘要

甲烷干重整（DRM）反应能够将CO

和CH

两种主要温室气体高效转化为H

和CO，从而实现资源化利用，具有重要的研究意义。Ni基催化剂因具有成本较低和活性较高的特点备受关注，但易因积炭导致失活，这一问题亟待解决。采用硅溶胶辅助溶液燃烧法制备了具有三维介孔结构的Ni-ZrO

催化剂，并将其应用于低温DRM反应。通过N

吸/脱附、XRD、H

-TPR、TEM和TG-DTA等多种表征手段，系统研究了催化剂结构以及Ni含量（质量分数，下同）和反应温度对催化剂催化性能的影响，并与普通浸渍法及传统溶液燃烧法制备的催化剂进行了对比。结果表明，硅溶胶辅助溶液燃烧法制备的催化剂具有较大的比表面积和稳定的三维介孔结构，并展现出更强的金属-载体相互作用。在催化性能方面，Ni含量对催化剂抗积炭性能和催化活性均具有显著影响。随着Ni含量的增大，催化剂的积炭倾向显著增强。在温度为600 °C、空速为135000 mL/(g·h)下进行20 h低温DRM反应后，具有三维介孔结构的1%Ni-ZrO

-CSC催化剂的CH

和CO

转化率分别维持在31%和38%，

(CO)稳定在0.45，且未观察到积炭生成，表明其具有优异的抗积炭性能。

Abstract

The dry reforming of methane (DRM) reaction efficiently converts two major greenhouse gases

and CH

into H

and CO

thereby achieving resource utilization and holding significant research value. Ni-based catalysts have garnere

d attention due to their low cost and high activity

but their deactivation caused by coking remains a pressing issue. Three-dimensional mesoporous Ni-ZrO

catalysts were prepared by colloidal silica-assisted solution combustion method and applied to low-temperature DRM reaction. Characterizations including N

adsorption/desorption

XRD

-TPR

TEM

and TG-DTA were conducted to systematically investigate the structures and the effects of Ni contents (mass fraction

the same below) and reaction temperatures on catalytic performance of catalysts. Comparisons were made with catalysts prepared via ordinary impregnation method and traditional solution combustion method. The results indicate that the catalysts prepared by colloidal silica-assisted solution combustion method exhibit larger specific surface areas

stable three-dimensional mesoporous structures

and have strong metal-support interactions. Regarding catalytic performance

Ni contents significantly affect both anti-coking performances and catalytic activities. As the Ni contents increase

the tendency of catalysts for coking becomes more pronounced. After a 20 h low-temperature DRM reaction at the temperature of 600 ℃ and space velocity of 135000 mL/(g·h)

the three-dimensional mesoporous 1%Ni-ZrO

-CSC catalyst maintains CH

and CO

conversion rates of 31% and 38%

respectively. The

(CO) stabilizes at 0.45

and no coking is observed

demonstrating 1%Ni-ZrO

-CSC’s excellent resistance to coking.

关键词

Keywords

references

ZHU H B , CHEN H C , ZHANG M H , et al . Recent advances in promoting dry reforming of methane using nickel-based catalysts [J ] . Catalysis Science & Technology , 2024 , 14 ( 7 ): 1712 - 1729 .

李真薇 , 李玉峰 , 陈杰 , 等 . 载体形貌调控Ni基催化剂甲烷干重整反应性能的研究 [J ] . 低碳化学与化工 , 2024 , 49 ( 8 ): 57 - 65 .

LI Z W ， LI Y F , CHEN J , et al . Study on reaction performance in methane dry reforming over Ni-based catalysts regulated by support morphologies [J ] . Low-Carbon Chemistry and Chemical Engineering , 2024 , 49 ( 8 ): 57 - 65 .

ZONG Z Y , CAI G P , TABBARA M , et al . CO 2 -negative fuel production using low-CO 2 electricity: Syngas from a combination of methane pyrolysis and dry reforming with techno-economic analysis [J ] . Energy Conversion and Management , 2023 , 277 : 116624 .

SHI Y , TIAN X Y , DENG Z Y , et al . Review and outlook of confined Ni catalysts for the dry reforming of methane reaction [J ] . Energy & Fuels , 2024 , 38 ( 3 ): 1633 - 1656 .

SHEN D Y , LI Z , SHAN J , et al . Synergistic Pt-CeO 2 interface boosting low temperature dry reforming of methane [J ] . Applied Catalysis B: Environment and Energy , 2022 , 318 : 121809 .

JIMENEZ J D , BETANCOURT L E , DANIELIS M , et al . Identification of highly selective surface pathways for methane dry reforming using mechanochemical synthesis of Pd-CeO 2 [J ] . ACS Catalysis , 2022 , 12 ( 20 ): 12809 - 12822 .

ANDROULAKIS A , YENTEKAKIS I , PANAGIOTOPOULOU P . Dry reforming of methane over supported Rh and Ru catalysts: Effect of the support (Al 2 O 3 , TiO 2 , ZrO 2 , YSZ) on the activity and reaction pathway [J ] . International Journal of Hydrogen Energy , 2023 , 48 ( 87 ): 33886 - 33902 .

WANG F G , WANG Y , ZHANG L J , et al . Performance enhancement of methane dry reforming reaction for syngas production over Ir/Ce 0.9 La 0.1 O 2 -nanorods catalysts [J ] . Catalysis Today , 2020 , 355 : 502 - 511 .

TORREZ-HERRERA J J , KORILI S A , GIL A . Recent progress in the application of Ni-based catalysts for the dry reforming of methane [J ] . Catalysis Reviews , 2021 , 65 ( 4 ): 1300 - 1357 .

WANG Y , YAO L , WANG S H , et al . Low-temperature catalytic CO 2 dry reforming of methane on Ni-based catalysts: A review [J ] . Fuel Processing Technology , 2018 , 169 : 199 - 206 .

SHEN D Y , WANG J , BAI Y , et al . Carbon-confined Ni based catalyst by auto-reduction for low-temperature dry reforming of methane [J ] . Fuel , 2023 , 339 : 127409 .

REN Y , MA Y Y , MO W L , et al . Research progress of carbon deposition on Ni-based catalyst for CO 2 -CH 4 reforming [J ] . Catalysts , 2023 , 13 ( 4 ): 647 .

HAUG L , THURNER C , BEKHEET M F , et al . Pivotal role of Ni/ZrO 2 phase boundaries for coke-resistant methane dry reforming catalysts [J ] . Catalysts , 2023 , 13 ( 5 ): 804 .

DAOURA O , FORNASIERI G , BOUTROS M , et al . One-pot prepared mesoporous silica SBA-15-like monoliths with embedded Ni particles as selective and stable catalysts for methane dry reforming [J ] . Applied Catalysis B: Environmental , 2021 , 280 : 119417 .

BAHARUDIN L , RAHMAT N , OTHMAN N H , et al . Formation, control, and elimination of carbon on Ni-based catalyst during CO 2 and CH 4 conversion via dry reforming process: A review [J ] . Journal of CO 2 Utilization , 2022 , 61 : 102050 .

SHARIFIANJAZI F , ESMAEILKHANIAN A , BAZLI L , et al . A review on recent advances in dry reforming of methane over Ni- and Co-based nanocatalysts [J ] . International Journal of Hydrogen Energy , 2022 , 47 ( 100 ): 42213 - 42233 .

TATHOD A P , HAYEK N , SHPASSER D , et al . Mediating interaction strength between nickel and zirconia using a mixed oxide nanosheets interlayer for methane dry reforming [J ] . Applied Catalysis B: Environmental , 2019 , 249 : 106 - 115 .

LIU S , DUN C C , SHAH M , et al . Producing ultrastable Ni-ZrO 2 nanoshell catalysts for dry reforming of methane by flame synthesis and Ni exsolution [J ] . Chem Catalysis , 2022 , 2 ( 9 ): 2262 - 2274 .

SHAO J L , LI C , FEI Z Y , et al . MOFs-derived Ni@ZrO 2 catalyst for dry reforming of methane: Tunable metal-support interaction [J ] . Molecular Catalysis , 2024 , 558 : 114028 .

DANGHYAN V , KUMAR A , MUKASYAN A , et al . An active and stable NiOMgO solid solution based catalysts prepared by paper assisted combustion synthesis for the dry reforming of methane [J ] . Applied Catalysis B: Environmental , 2020 , 273 : 119056 .

JIN H Y , LIU Y Q , HUANG L Z , et al . Three-dimensional mesoporous Ni-CeO 2 catalyst for dry reforming of methane [J ] . Catalysts , 2024 , 14 ( 5 ): 291 .

ZHAO K C , WANG W H , LI Z H . Highly efficient Ni/ZrO 2 catalysts prepared via combustion method for CO 2 methanation [J ] . Journal of CO 2 Utilization , 2016 , 16 : 236 - 244 .

GE F J , ZHU J , DU X H , et al . Constructing the highly efficient Ni/ZrO 2 /SiO 2 catalyst by a combustion-impregnation method for low-temperature CO 2 methanation [J ] . Journal of Environmental Chemical Engineering , 2022 , 10 ( 5 ): 108476 .

VOSKANYAN A A , CHAN K Y , LI C Y V . Colloidal solution combustion synthesis: Toward mass production of a crystalline uniform mesoporous CeO 2 catalyst with tunable porosity [J ] . Chemistry of Materials , 2016 , 28 ( 8 ): 2768 - 2775 .

OMAROV S O , SLADKOVSKIY D A , MARTINSON K D , et al . Influence of the initial state of ZrO 2 on genesis, activity and stability of Ni/ZrO 2 catalysts for steam reforming of glycerol [J ] . Applied Catalysis A: General , 2021 , 616 : 118098 .

ZHOU R F , MAHINPEY N . A review on catalyst development for conventional thermal dry reforming of methane at low temperature [J ] . The Canadian Journal of Chemical Engineering , 2023 , 101 ( 6 ): 3180 - 3212 .

DAS S , ASHOK J , BIAN Z , et al . Silica-ceria sandwiched Ni core-shell catalyst for low temperature dry reforming of biogas: Coke resistance and mechanistic insights [J ] . Applied Catalysis B: Environmental , 2018 , 230 : 220 - 236 .

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Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO2 catalysts

DOI：10.12434/j.issn.2097-2547.20250005

摘要

Abstract

关键词

Keywords

references

Performance study of dry reforming of methane over three-dimensional mesoporous Ni-ZrO₂ catalysts