Noble metal (Pt, Pd and Rh) promoted Ni-Co/Mg(Al)O catalysts for steam reforming of tar impurities from biomass gasification

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-05-22 DOI:10.1016/j.jcat.2024.115567

Ask Lysne, Ida Saxrud, Rémi L.G. Snidaro, Edd A. Blekkan

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Abstract

Steam reforming is a promising approach to remove biomass gasification tar impurities. Noble metal promotion (Pt/Pd/Rh), Ni+Co loading (20–40 wt%) and calcination temperature (600–800 °C) effects were investigated with hydrotalcite-derived Ni-Co/Mg(Al)O catalysts for bio-syngas tar steam reforming. Fresh catalysts were characterized by XRD, ICP-MS, XRF, N₂-physisorption, H₂-chemisorption and TPR. Small-diameter metal particles were achieved (5.1–5.8 nm) below a Ni+Co loading threshold (above 30 wt%). Model bio-syngas activity tests were performed (CH₄/H₂/CO/CO₂ molar ratio = 10/35/25/25, 700 °C, steam-to-carbon = 3.0) with and without tar addition (toluene/1-methylenaphthalene, 10 g/Nm³). Tar elimination was achieved with all samples. Enhanced reforming activity accompanied by strong tar active site inhibition effects were found for the Rh promoted catalyst. Noble metal promoted samples were effectively reduced in the bio-syngas environment (H₂/CO/CH₄) without any pre-reduction (in situ activation by the action of the syngas) with Rh > Pt > Pd. Coke characterization was conducted with TPO-MS and Raman spectroscopy. High-dispersion 20NiCo/30NiCo samples were strongly deactivated through active site inhibition and coke formation. High-temperature calcination (800 °C) reduced the deactivation effects of the coke deposition, attributed to enhanced Mg(Al)O-assisted coke gasification.

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贵金属（铂、钯和铑）促进的 Ni-Co/Mg(Al)O 催化剂用于生物质气化焦油杂质的蒸汽转化

蒸汽转化是去除生物质气化焦油杂质的一种可行方法。研究了水滑石衍生 Ni-Co/Mg(Al)O 催化剂在生物合成气焦油蒸汽转化中贵金属促进（Pt/Pd/Rh）、Ni+Co 负载（20-40 wt%）和煅烧温度（600-800 °C）的影响。对新鲜催化剂进行了 XRD、ICP-MS、XRF、N2-物理吸附、H2-化学吸附和 TPR 表征。在 Ni+Co 负载阈值（高于 30 wt%）以下实现了小直径金属颗粒（5.1-5.8 nm）。在添加和不添加焦油（甲苯/1-甲基萘，10 g/Nm3）的情况下，进行了生物合成气活性模型试验（CH4/H2/CO/CO2 摩尔比 = 10/35/25/25，700 °C，蒸汽碳比 = 3.0）。所有样品都能消除焦油。在提高重整活性的同时，还发现 Rh 促进的催化剂具有很强的焦油活性位点抑制作用。贵金属促进的样品在生物合成气环境（H2/CO/CH4）中有效地还原了 Rh > Pt > Pd，而无需任何预还原（通过合成气的作用进行原位活化）。焦炭的表征是通过 TPO-MS 和拉曼光谱进行的。高分散度的 20NiCo/30NiCo 样品通过活性位点抑制和焦炭形成被强烈失活。高温煅烧（800 °C）降低了焦炭沉积的失活效应，这归因于 Mg(Al)O 辅助焦炭气化的增强。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.