Effect of Ni/Co ratio on Ce-Sc-ZrO2 catalysts for selective H2 production via methane partial oxidation

IF 5.8 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of Saudi Chemical Society Pub Date : 2024-10-05 DOI:10.1016/j.jscs.2024.101948

Norah Alwadai , Ahmed S. Al-Fatesh , Kenit Acharya , Abdulaziz A.M. Abahussain , Salma A. Al-Zahrani , Anis H. Fakeeha , Naif Alarifi , Khaled M. Banabdwin , Ahmed A. Ibrahim , Rawesh Kumar

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Abstract

Partial oxidation of methane (POM) is a promising route for hydrogen production, and achieving a high H₂ yield with an H₂/CO ratio >3 is highly appealing. Optimization of Ni/Co ratios over Ce-Sc-ZrO₂ (CSZ) is investigated for POM reaction and characterized by X-ray diffraction, Raman spectroscopy, temperature-programmed reduction/oxidation/desorption, and transmission electron microscopy. The active site derived from the reduction of “strongly interacted NiO” is responsible for the dissociation of C–H (of CH₄), resulting high activity towards POM. 5Ni/CSZ has the highest amount of such active sites and attains the highest activity. 5Co/CSZ catalyst has cobalt-based active sites, and there is an inert carbon deposit during the reaction, causing the least activity. 3.75 wt% Ni and 1.25 wt% Co combination over CSZ support surges the highest density of basicity, oxide vacancy, and adequate amount of active sites derived from “strongly interacted NiO”. The active sites with enhanced metal-support interaction are further grown under exposure to oxidizing gas (O₂) and reducing gas (H₂) during the POM reaction. The highest density of basicity and oxide vacancy involves more CO₂ and H₂O in the sequential oxidation of CH₄ under indirect pathways. The exclusive involvement of indirect pathways of POM and inhibition of hydrogen consuming reaction (like reverse water gas shift reaction) over 3.75Ni1.25Co/CSZ results into 48 % H₂ yield and 3.26 H₂/CO ratio up to 24 h time on stream at 600 °C. The H₂ yield doubles to ∼97 %, and the H₂/CO ratio comes close to 2 over 3.75Ni1.25Co/CSZ catalyst at 900 °C.

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镍/钴比对通过甲烷部分氧化选择性生产 H2 的 Ce-Sc-ZrO2 催化剂的影响

甲烷部分氧化（POM）是一种前景广阔的制氢途径，以 H2/CO 比率 >3 获得较高的 H2 产率极具吸引力。研究人员通过 X 射线衍射、拉曼光谱、温度编程还原/氧化/解吸和透射电子显微镜，对 Ce-Sc-ZrO2 (CSZ) 上的 Ni/Co 比率进行了优化，以用于 POM 反应。强相互作用氧化镍 "还原产生的活性位点负责解离（CH4 的）C-H，从而对 POM 具有高活性。5Ni/CSZ 催化剂中这种活性位点的数量最多，活性也最高。5Co/CSZ 催化剂具有钴基活性位点，在反应过程中会有惰性碳沉积，因此活性最低。CSZ 载体上 3.75 wt% Ni 和 1.25 wt% Co 的组合具有最高的碱度密度、氧化物空位和充足的 "强相互作用 NiO "活性位点。在 POM 反应过程中，在氧化性气体（O2）和还原性气体（H2）的作用下，金属-支撑相互作用增强的活性位点进一步增长。碱度和氧化物空位密度最高时，在间接途径下的 CH4 顺序氧化过程中会涉及更多的 CO2 和 H2O。在 3.75Ni1.25Co/CSZ 上，POM 间接途径的完全参与和对耗氢反应（如反向水气变换反应）的抑制，使得在 600 °C 下的 24 小时内，H2 产率达到 48%，H2/CO 比率达到 3.26。在 900 °C 时，3.75Ni1.25Co/CSZ 催化剂的 H2 产率翻了一番，达到 97%，H2/CO 比率接近 2。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Journal of Saudi Chemical Society CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

8.90

自引率

1.80%

发文量

120

审稿时长

38 days

期刊介绍： Journal of Saudi Chemical Society is an English language, peer-reviewed scholarly publication in the area of chemistry. Journal of Saudi Chemical Society publishes original papers, reviews and short reports on, but not limited to: •Inorganic chemistry •Physical chemistry •Organic chemistry •Analytical chemistry Journal of Saudi Chemical Society is the official publication of the Saudi Chemical Society and is published by King Saud University in collaboration with Elsevier and is edited by an international group of eminent researchers.