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CO2 Methanation on Ni Catalysts Supported over Activated Carbons Derived from Cork Waste
Energy & Fuels ( IF 5.2 ) Pub Date : 2023-06-02 , DOI: 10.1021/acs.energyfuels.3c00908
Filipe Mateus 1 , Paula Teixeira 1 , José M. Lopes 1 , Carlos Henriques 1 , Carmen Bacariza 1
Energy & Fuels ( IF 5.2 ) Pub Date : 2023-06-02 , DOI: 10.1021/acs.energyfuels.3c00908
Filipe Mateus 1 , Paula Teixeira 1 , José M. Lopes 1 , Carlos Henriques 1 , Carmen Bacariza 1
Affiliation
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Activated carbons (ACs) derived from cork wastes were for the first time used as supports for CO2 methanation catalysts. Cork wastes (natural-N and processed-P) were physically activated under N2/H2O(v) atmosphere at 800 °C to obtain the corresponding AC supports (ACN and ACP, respectively). Ni and Ni-CeO2 catalysts were prepared by loading the ACs with 15 wt % Ni (Ni/AC) or 15 wt % Ni and 15 wt % Ce (NiCe/AC) by incipient wetness impregnation or co-impregnation, respectively, using 2-propanol as the solvent. For comparison purposes, a commercial activated carbon (ACC) was impregnated with the same metals and loadings. The catalysts were characterized by N2 and CO2 sorption, XRD, TGA, SEM, and TEM, and finally tested at atmospheric pressure under CO2 methanation conditions (86 100 mL·h–1·gcat–1, H2/CO2 = 4:1). Microporous activated carbons with high surface areas (757–903 m2·g–1) were obtained from natural and processed cork wastes. While nickel was incorporated as Ni0 over the materials, CeO2 phases were detected on Ni-CeO2 catalysts. The incorporation of these metal species over the activated carbons induced a decrease of the textural properties, while the affinity toward CO2 was promoted by CeO2. In terms of average Ni0 particle sizes, while the smallest ones were detected on Ni/ACC (8 nm) for Ni/AC samples, the addition of CeO2 led to a remarkable decrease of this parameter on cork-derived materials (from 20 to 7 nm and from 33 to 16 nm on ACN and ACP, respectively). Higher CH4 yields were exhibited by CeO2-containing catalysts, with relative CH4 yield increases of 210–670% using Ni samples as the basis being observed. This was ascribed to CeO2’s ability to activate CO2 and promote Ni0 dispersion. The best results (CH4 yield of 73% at 400 °C) were obtained for the NiCe/ACN catalyst, its performance being similar to or higher than that reported in the literature for similar systems, thus motivating further development and optimization of these materials for CO2 methanation.
中文翻译：
软木废料活性炭负载 Ni 催化剂上的 CO2 甲烷化
源自软木废料的活性炭 (AC) 首次用作 CO 2甲烷化催化剂的载体。软木废料（天然 N 和加工过的 P）在 N 2 /H 2 O (v)气氛下于 800 °C 下进行物理活化，以获得相应的 AC 支持（分别为 AC N和 AC P）。Ni 和 Ni-CeO 2催化剂是通过初湿浸渍或共浸渍分别用 15 wt% Ni (Ni/AC) 或 15 wt% Ni 和 15 wt% Ce (NiCe/AC) 负载活性炭制备的，使用2-丙醇作为溶剂。为了进行比较，商业活性炭（AC C) 浸渍了相同的金属和负载。通过N 2和CO 2吸附、XRD、TGA、SEM和TEM对催化剂进行了表征，最后在CO 2甲烷化条件（86 100 mL·h –1 ·g cat –1 , H 2 /CO 2 = 4:1)。具有高表面积 (757–903 m 2 ·g –1 ) 的微孔活性炭是从天然和加工过的软木废料中获得的。当镍以 Ni 0 的形式结合在材料上时，在 Ni-CeO 2上检测到CeO 2相催化剂。在活性炭上掺入这些金属物质导致结构特性下降，而CeO 2促进了对 CO 2的亲和力。就平均 Ni 0粒径而言，虽然最小的是在 Ni/AC C (8 nm) 上检测到的 Ni/AC 样品，但添加 CeO 2导致软木衍生材料的该参数显着降低（来自AC N和 AC P上分别为 20 至 7 nm 和 33 至 16 nm ）。含 CeO 2的催化剂表现出较高的 CH 4产率，相对 CH 4使用 Ni 样品作为观察的基础，产量增加了 210-670%。这归因于 CeO 2激活 CO 2并促进 Ni 0分散的能力。NiCe/AC N催化剂获得了最好的结果（在 400 °C 时 CH 4产率为 73%） ，其性能类似于或高于文献中针对类似系统报道的性能，从而推动了这些催化剂的进一步开发和优化CO 2甲烷化原料。
更新日期：2023-06-02
中文翻译：
软木废料活性炭负载 Ni 催化剂上的 CO2 甲烷化
源自软木废料的活性炭 (AC) 首次用作 CO 2甲烷化催化剂的载体。软木废料（天然 N 和加工过的 P）在 N 2 /H 2 O (v)气氛下于 800 °C 下进行物理活化，以获得相应的 AC 支持（分别为 AC N和 AC P）。Ni 和 Ni-CeO 2催化剂是通过初湿浸渍或共浸渍分别用 15 wt% Ni (Ni/AC) 或 15 wt% Ni 和 15 wt% Ce (NiCe/AC) 负载活性炭制备的，使用2-丙醇作为溶剂。为了进行比较，商业活性炭（AC C) 浸渍了相同的金属和负载。通过N 2和CO 2吸附、XRD、TGA、SEM和TEM对催化剂进行了表征，最后在CO 2甲烷化条件（86 100 mL·h –1 ·g cat –1 , H 2 /CO 2 = 4:1)。具有高表面积 (757–903 m 2 ·g –1 ) 的微孔活性炭是从天然和加工过的软木废料中获得的。当镍以 Ni 0 的形式结合在材料上时，在 Ni-CeO 2上检测到CeO 2相催化剂。在活性炭上掺入这些金属物质导致结构特性下降，而CeO 2促进了对 CO 2的亲和力。就平均 Ni 0粒径而言，虽然最小的是在 Ni/AC C (8 nm) 上检测到的 Ni/AC 样品，但添加 CeO 2导致软木衍生材料的该参数显着降低（来自AC N和 AC P上分别为 20 至 7 nm 和 33 至 16 nm ）。含 CeO 2的催化剂表现出较高的 CH 4产率，相对 CH 4使用 Ni 样品作为观察的基础，产量增加了 210-670%。这归因于 CeO 2激活 CO 2并促进 Ni 0分散的能力。NiCe/AC N催化剂获得了最好的结果（在 400 °C 时 CH 4产率为 73%） ，其性能类似于或高于文献中针对类似系统报道的性能，从而推动了这些催化剂的进一步开发和优化CO 2甲烷化原料。
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