Pyrolysis-catalytic gasification of plastic waste for hydrogen-rich syngas production with hybrid-functional Ni-CaOCa2SiO4 catalyst

Tian Heng Qin , Guozhao Ji , Boyu Qu , Alan J McCue , Shaoliang Guan , Jos Derksen , Ye Shui Zhang
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Abstract

The production of H2-rich syngas from pyrolysis-catalytic gasification of plastic waste bottles has been investigated. The hybrid-functional materials consisting of Ni as catalyst, CaO as CO2 sorbent and Ca2SiO4 as a polymorphic active spacer were synthesized. The different parameters (Ni loading, temperature, N2 flow rate and feedstock-to-catalyst ratio) have been investigated to optimise the H2 production. The catalysts were analysed by N2 physisorption, scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Temperature-programmed reduction (TPR) and in-situ Transmission Electron Microscopy (TEM). Temperature-programmed oxidation (TPO) was used to analyse the carbon formation on the used catalysts. The highest H2 production of 59.15 mmol g-1of plastic was obtained in the presence of a catalyst with 20 wt.% Ni loading, which amounts to H2 purity as high as 54.2 vol% in gas production. Furthermore, 90.63 mmol g-1of plastic of syngas was produced by increasing the feedstock-to-catalyst ratio to 4:1, yielding 84.4 vol.% of total gas product (53.1 vol.% of H2 and 31.3 vol.% of CO, respectively). The Ni-CaOCa2SiO4 hybrid-functional material is a very promising catalyst in the pyrolysis-catalytic gasification process by capturing CO2 as it is produced, therefore shifting the water gas shift (WGS) reaction to enhance H2 production from plastic waste. Detailed elucidation of the roles of each component at the microscale during the catalytic process was also provided through in-situ TEM analysis. The finding could guide the industry for future large-scale application to convert abundant plastic waste into H2-rich syngas, therefore contributing to the global ‘net zero’ ambition.

Abstract Image

混合功能Ni-CaOCa2SiO4催化剂催化塑料废弃物热解气化富氢合成气研究
研究了废塑料瓶热解催化气化生产富h2合成气的工艺。合成了以Ni为催化剂、CaO为CO2吸附剂、Ca2SiO4为多态活性间隔剂的杂化功能材料。研究了不同的参数(Ni负载、温度、N2流量和原料-催化剂比)来优化H2的产量。采用N2物理吸附、扫描电镜(SEM)、能谱(EDS)、x射线衍射(XRD)、x射线光电子能谱(XPS)、程序升温还原(TPR)和原位透射电镜(TEM)对催化剂进行了分析。采用程序升温氧化法(TPO)对催化剂的碳生成进行了分析。在含镍量为20wt .%的催化剂下,塑料的H2产量最高,为59.15 mmol g-1,产气H2纯度高达54.2% vol%。将原料与催化剂的比例提高到4:1时,合成气的塑料产量为90.63 mmol g-1,产气量为84.4 vol.% (H2为53.1 vol.%, CO为31.3 vol.%)。Ni-CaOCa2SiO4混合功能材料是一种非常有前途的催化剂,它可以在产生二氧化碳时捕获二氧化碳,从而改变水煤气转换(WGS)反应,从而提高塑料废物的H2产量。通过原位透射电镜分析,在微观尺度上详细阐明了各组分在催化过程中的作用。这一发现可以指导该行业未来大规模应用,将大量塑料废物转化为富含h2的合成气,从而为全球“净零”目标做出贡献。
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