<br>镍基催化剂焦油催化重整碳纳米管积碳机理研究,Journal of Environmental Management

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镍基催化剂焦油催化重整碳纳米管积碳机理研究
Journal of Environmental Management ( IF 8.0 ) Pub Date : 2024-06-04 , DOI: 10.1016/j.jenvman.2024.121349
Rujiao Jiang ₁ , Baojun Yi ₂ , Qi Wei ₁ , Zhi He ₁ , Zhengshuai Sun ₁ , Jiayi Yang ₁ , Wenbin Hua ₁

Affiliation

使用镍基催化剂是通过催化裂化消除焦油的常用方法。积碳是 Ni/ZSM-5 催化剂失活的主要原因，其中丝状 MWCNT 是积碳的主要形式。本研究研究了生物质焦油催化过程中碳纳米管的形成和演化，以探讨碳沉积背后的机制。通过立式炉研究了9Ni/10MWCNTs/81ZSM-5对甲苯重整的影响。通过气相色谱分析评估焦油催化产生的气体。并对催化剂的理化结构、性能和催化性能进行了测试。热重分析用于评估催化剂表面碳的积累和氧化反应性。对焦油催化催化剂失活过程中积碳的机理进行了分析。结果表明，9Ni/91ZSM-5 的甲苯转化率高达 60.49%，但也经历了快速且大量的碳沉积，高达 52.69%。碳主要以弯曲丝的形式沉积在催化剂的表面和孔道上。在某些情况下，尖端生长发生在碳沉积和镍共存的地方。此外，由于积碳，比表面积和微孔体积都有不同程度的减少。随着时间的增加，催化剂表面碳沉积量增加至62.81%，逐渐接近饱和，催化剂整体性能趋于稳定。这种情况导致甲苯分子从催化剂内的活性位点脱离，阻碍气体释放，从而导致催化活性降低和进一步的碳沉积。它既为新型催化剂的开发提供了基础，又为实际焦油减少和去除提供了经济可行的解决方案。

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Study on the mechanism of carbon nanotube-like carbon deposition in tar catalytic reforming over Ni-based catalysts

The use of Ni-based catalysts is a common method for eliminating tar through catalytic cracking. Carbon deposition is the main cause of deactivation in Ni/ZSM-5 catalysts, with filamentous MWCNTs being the primary form of carbon deposits. This study investigates the formation and evolution of CNTs during the catalytic process of biomass tar to explore the mechanism behind carbon deposition. The effect of the 9Ni/10MWCNTs/81ZSM-5 on toluene reforming was investigated through a vertical furnace. Gases produced by tar catalysis were evaluated through GC analysis. The physicochemical structure, properties and catalytic performance of the catalyst were also tested. TG analysis was used to assess the accumulation and oxidation reactivity of carbon on the catalyst surface. An analysis was conducted on the mechanism of carbon deposition during catalyst deactivation in tar catalysis. The results showed that the 9Ni/91ZSM-5 had a superior toluene conversion of 60.49%, but also experienced rapid and substantial carbon deposition up to 52.69%. Carbon is mainly deposited as curved filaments on both the surface and pore channels of the catalyst. In some cases, tip growth occurs where both carbon deposition and Ni coexist. Furthermore, specific surface area and micropore volume are reduced to varying degrees due to carbon deposition. With the time increased, the amount of carbon deposited on the catalyst surface increased to 62.81%, which gradually approached saturation, and the overall performance of the catalyst was stabilized. This situation causes toluene molecules to detach from the active sites within the catalyst, hindering gas release, which leads to reduced catalytic activity and further carbon deposition. It provides both a basis for the development of new catalysts and an economically feasible solution for practical tar reduction and removal.

更新日期：2024-06-04

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