打破固态共磨实现的镍负载-可重复性-分散度依赖性

IF 4.3 3区 工程技术 Q2 ENGINEERING, CHEMICAL Frontiers of Chemical Science and Engineering Pub Date : 2024-09-05 DOI:10.1007/s11705-024-2499-9
Yong-Shan Xiao, Min-Li Zhu, Han-Qing Ge, Zhong-Wen Liu
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引用次数: 0

摘要

负载-分散-可重复性依赖性一直是开发高性能支撑金属催化剂的最关键问题之一。在此,通过共同研磨含模板的 OMA 和 Ni(NO3)2-6H2O 的混合物,制备了有序介孔氧化铝(OMA)上的氧化镍含量高达 40 wt %。表征结果证实,即使氧化镍的含量高达 40 wt %,OMA 的介孔结构仍得以保留。更重要的是,当 NiO 的负载量从 20 wt % 增加到 40 wt % 时,Ni/OMA 催化剂的还原度、分散度和平均粒径分别保持在 91.0%、13.5% 和 4.0-5.0 nm。以 CO 甲烷化为模型反应对催化剂进行了评估,在 300 °C 下,所有 Ni/OMA 催化剂都达到了 24.0 h-1 的高翻转频率。对于氧化镍负载量最高为 40 wt % 的催化剂(40Ni/OMA),300 °C 时的低温活性以甲烷的时空产率为指标(over (325.8 (text{mol}_{text\{CH}_{4}}),同时催化剂在 600 °C 的苛刻反应条件和 240000 mL-g-1-h-1 的极高气体时空速度下运行了 120 h,没有观察到失活现象。通过这些重要成果,这项工作打破了负载-分散-可重复性的依赖关系,在苛刻的反应条件下稳定了镍纳米颗粒,为合理、可控地设计支撑镍催化剂铺平了道路。
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Breaking the Ni loading-reducibility-dispersion dependence achieved by solid-state co-grinding

The loading-dispersion-reducibility dependence has always been one of the most critical issues in the development of high-performance supported metal catalysts. Herein, up to 40 wt % NiO over ordered mesoporous alumina (OMA) was prepared by co-grinding the hybrid of template-containing OMA and Ni(NO3)2·6H2O. Characterization results confirmed that the OMA mesostructure was still preserved even after loading NiO at a content as high as 40 wt %. More importantly, the reduction extent, dispersion, and average particle size of the Ni/OMA catalysts were maintained at ⩾ 91.0%, ∼13.5%, and ∼4.0–5.0 nm, respectively, when the NiO loading was increased from 20 to 40 wt %. The catalysts were evaluated for the CO methanation as a model reaction, and the similarly high turnover frequency of 24.0 h−1 was achieved at 300 °C for all of the Ni/OMA catalysts. For the catalyst with the highest NiO loading of 40 wt % (40Ni/OMA), the low-temperature activity at 300 °C indexed by the space-time yield of methane (over \(325.8\ \text{mol}_{\text{CH}_{4}}\cdot \ {\text{kg}_{\text{cat}}}^{-1}\cdot \mathrm{h}^{-1}\)) was achieved, while the catalyst was operated without an observable deactivation for a time on stream of 120 h under severe reaction conditions of 600 °C and a very high gas hourly space velocity of 240000 mL·g−1·h−1. With these significant results, this work paves the way for a rational and controllable design of supported Ni catalysts by breaking the loading-dispersion-reducibility dependence and stabilizing Ni nanoparticles under harsh reaction conditions.

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来源期刊
CiteScore
7.60
自引率
6.70%
发文量
868
审稿时长
1 months
期刊介绍: Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.
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