Jin Lv, Youhe Wang, Junjie Liu, Zhichao Zhang, Yu Ma, Ziyi Zhou, Yuqing Ouyang, Jie Zhong, Xiang Rao, Hongman Sun, Xiaoyun Xiong, Qingxun Hu, Guofeng Zhao, Zifeng Yan
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引用次数: 0
摘要
甲烷干重整(DRM)可同时将两种重要的温室气体 CH4 和 CO2 转化为高价值的合成气。然而,镍基催化剂在高温下烧结和碳沉积导致的催化剂失活是干转化甲烷工业化亟待解决的重要问题。在此,我们提出了一种用于 DRM 反应的分层 Ni-La@S-1 催化剂,该催化剂具有较高的抗烧结/积炭能力,可提高 DRM 的稳定性。首先将 La 和 Ni 硝酸盐研磨到 SBA-15 的孔隙中,然后进行 N2 处理;然后采用独特的模板辅助-均匀分散策略对样品进行重结晶,从而获得分层 Ni-La@S-1 催化剂。该策略实现了稳定的 Ni-La 双金属纳米颗粒在 S-1 中的均匀封装,且负载量高,在 700 °C 和 36,000 mL-g-1-h-1 温度条件下表现出较高的 DRM 活性和稳定性。此外,La 的加入促进了 CO2 生成双齿碳酸盐(DRM 的关键中间体),从而大大改善了 Ni 催化剂中的碳沉积。这项工作为定制工业 DRM 催化剂提供了很有前景的线索。
Dry-gel synthesis of hierarchical Ni-La@S-1 catalysts with stabilized Ni-La bimetals nanoparticles for dry reforming of methane
Dry reforming of methane (DRM) can simultaneously convert two critical greenhouse gases CH4 and CO2 into high-value syngas. However, the catalyst deactivation caused by sintering and carbon deposition of Ni-based catalysts at high temperature is a significant problem to be solved for DRM industrialization. Herein, we represent a hierarchical Ni-La@S-1 catalyst for DRM reaction, showing high anti-sintering/coke capacity to improve DRM stability. The La and Ni nitrates were first grinded into the pores of SBA-15 followed by N2-treatment; the sample was then recrystallized by a unique template assisted-uniformly dispersed strategy to obtain the hierarchical Ni-La@S-1 catalyst. This strategy achieves uniform encapsulation of stabilized Ni-La bimetallic nanoparticles in S-1 with high loading, exhibiting high DRM activity and stability at 700 °C and 36,000 mL·g−1·h−1. Moreover, La addition promoted CO2 to form bidentate carbonate, a critical intermediate in DRM, which greatly ameliorated carbon deposition in Ni catalysts. This work offers promising clue for tailoring the industrial DRM catalysts.
期刊介绍:
Nano Research is a peer-reviewed, international and interdisciplinary research journal that focuses on all aspects of nanoscience and nanotechnology. It solicits submissions in various topical areas, from basic aspects of nanoscale materials to practical applications. The journal publishes articles on synthesis, characterization, and manipulation of nanomaterials; nanoscale physics, electrical transport, and quantum physics; scanning probe microscopy and spectroscopy; nanofluidics; nanosensors; nanoelectronics and molecular electronics; nano-optics, nano-optoelectronics, and nano-photonics; nanomagnetics; nanobiotechnology and nanomedicine; and nanoscale modeling and simulations. Nano Research offers readers a combination of authoritative and comprehensive Reviews, original cutting-edge research in Communication and Full Paper formats. The journal also prioritizes rapid review to ensure prompt publication.