Key Takeaways & Executive Findings
- •• • The m-NCM-Al-sol catalyst, using inorganic aluminum sol as binder, achieves superior coating adhesion and forms a (Ni-Mg)AlxO4 composite structure via elemental diffusion, leading to the best catalytic activity and stability in DRM, with strong resistance to carbon deposition. • • In contrast, silica sol (Si-sol) binder results in coating cracks and detachment after calcination due to weak interactions, causing activity loss; organic binder (HEC) is oxidized and removed, yielding poor adhesion and severe particle agglomeration, resulting in the poorest performance. • • Coating adhesion strength, mesoporous confinement, and strong metal-support interactions (SMSI) are identified as key factors determining DRM performance; the Al-sol-derived mesoporous Al2O3 network effectively regulates charge transfer around metal sites, promoting C-H bond activation. • • Optimization of aluminum sol coating parameters (binder content, active component dosage, coating cycles) achieves a balance between coating thickness and mass transfer, enabling the integrated catalyst to exhibit excellent DRM performance.
Abstract
The CO2 dry reforming of methane (DRM) is pivotal for CO2 utilization within the dual-carbon framework, offering advantages in carbon reduction and value-added chemical production. However, shaped catalysts suitable for industrial-scale DRM remain limited. This work constructs a monolithic catalyst using honeycomb cordierite as the structural support, systematically investigating the effects of organic and inorganic binders on coating structure and catalytic performance. Comparative studies reveal that the active coating fabricated with inorganic aluminum sol exhibits a continuous uniform morphology and excellent adhesion strength. During high-temperature calcination, elemental diffusion within Al2O3 networks bridges the cordierite surface with active catalyst particles, forming a (Ni-Mg)AlxO4 composite structure. This creates robust metal-support interactions between active sites and the residual alumina matrix. The interconnected mesoporous framework provides superior pore confinement, contributing to strong coating adhesion, enhanced activity, and improved resistance to carbon deposition in the monolithic m-NCM-Al-sol catalyst. In contrast, coatings derived from inorganic silica sol suffer from detachment and activity loss due to heterogeneous surface structures and poor adhesion. Organic binders demonstrate inferior performance in macroscopic coating uniformity, adhesion strength, mesoporous confinement, and localized electronic effects, resulting in the poorest catalytic performance. By optimizing aluminum sol coating parameters—binder content, active component dosage, and coating cycles—a synergistic balance between coating thickness and mass transfer is achieved. The optimized catalyst demonstrates excellent DRM performance, providing insights for constructing high-performance shaped catalysts with cordierite coatings.
1. Introduction
Industrial dry reforming of methane (DRM) faces a critical bottleneck: conventional powder catalysts suffer from high pressure drop and poor heat transfer, hindering scale-up. Monolithic catalysts with honeycomb cordierite supports offer a solution, but their performance hinges on the integrity and structure of the catalytically active coating. Prior attempts using organic binders or silica sols have failed to achieve robust adhesion and stable mesoporous frameworks, leading to coating detachment, active site loss, and rapid deactivation. The lack of strong interfacial interactions between the coating and cordierite substrate exacerbates these issues under high-temperature reaction conditions.
This study systematically addresses these challenges by comparing organic and inorganic binders, demonstrating that an inorganic aluminum sol binder uniquely enables a continuous, strongly adhered coating. Through a dual diffusion mechanism during calcination, the Al2O3 network bridges the cordierite surface and active particles, forming a (Ni-Mg)AlxO4 composite with enhanced metal-support interactions. This structural reconstruction yields a mesoporous framework that confines metal particles, suppresses coke formation, and promotes C-H bond activation, resulting in superior DRM activity and stability. The findings provide a rational design strategy for industrial monolithic DRM catalysts.
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LIU Junyang, LIU Yupeng, XUE Rulin, LIU Lingji, ZHANG Chaoyang, LI Feng, LI Guoqiang, GENG Xiangdong, LI Lei, WANG Changzhen (2026). Binder-Mediated Regulation of Coating Structure over Monolithic Catalyst and Its Performance in CH4-CO2 Reforming. Journal of Fuel Chemistry and Technology. https://doi.org/10.1016/S1872-5813(26)60762-1
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Frequently Asked Questions
What is the failure mechanism of silica sol-based coatings under DRM conditions, and how does it compare to aluminum sol in terms of adhesion and catalytic stability?
Silica sol forms a rigid mesoporous network but lacks strong interactions with cordierite and active particles, leading to coating cracks and detachment after calcination. This compromises heat transfer and adhesion stability, causing activity loss. In contrast, aluminum sol undergoes elemental diffusion to form a (Ni-Mg)AlxO4 composite, creating robust interfacial bonding and superior anti-peeling capability, ensuring stable catalytic performance.
How does the mesoporous confinement effect of the Al-sol-derived coating suppress carbon deposition during DRM?
The interconnected mesoporous Al2O3 network physically confines Ni particles, preventing sintering and reducing the size of carbon growth sites. This confinement, combined with strong metal-support interactions, limits the formation of filamentous carbon, as evidenced by the catalyst's improved resistance to coking compared to Si-sol and organic binder counterparts.
What are the optimal coating parameters (binder content, active component dosage, coating cycles) for achieving high DRM performance, and what trade-offs exist?
The study optimized aluminum sol content, active component dosage, and coating cycles to balance coating thickness and mass transfer. While exact numerical values are not provided in the abstract, the optimization led to an integrated catalyst with excellent DRM performance, indicating that a synergistic balance is critical. Excessive coating thickness can hinder mass transfer, while insufficient thickness may reduce active site loading.
How does the (Ni-Mg)AlxO4 composite structure enhance catalytic activity compared to conventional Ni-based catalysts?
The (Ni-Mg)AlxO4 structure, formed via elemental diffusion, creates strong metal-support interactions that modify the electronic environment of Ni sites. This promotes C-H bond activation, as evidenced by enhanced activity. The strong interaction also stabilizes Ni against sintering, contributing to long-term stability.
What is the industrial significance of using honeycomb cordierite as a support, and how does the Al-sol coating address scalability challenges?
Honeycomb cordierite offers low pressure drop and high thermal conductivity, suitable for industrial fixed-bed reactors. The Al-sol coating ensures strong adhesion and uniform coverage, preventing active material loss during operation. This addresses scalability by providing a durable, high-performance monolithic catalyst that can be manufactured via dip-coating, a scalable process.
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