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发展镍和磁铁矿促进的碳化纤维素珠载双金属 Pd-Pt 催化剂用于水溶液中氯酸根离子的加氢。

Development of Nickel- and Magnetite-Promoted Carbonized Cellulose Bead-Supported Bimetallic Pd-Pt Catalysts for Hydrogenation of Chlorate Ions in Aqueous Solution.

机构信息

Institute of Chemistry, University of Miskolc, 3515 Miskolc-Egyetemváros, Hungary.

Higher Education Industry Cooperation Centre, University of Miskolc, 3515 Miskolc-Egyetemváros, Hungary.

出版信息

Int J Mol Sci. 2021 Oct 31;22(21):11846. doi: 10.3390/ijms222111846.

Abstract

Cellulose grains were carbonized and applied as catalyst supports for nickel- and magnetite-promoted bimetallic palladium- and platinum-containing catalysts. The bimetallic spherical aggregates of Pd and Pt particles were created to enhance the synergistic effect among the precious metals during catalytic processes. As a first step, the cellulose bead-based supports were impregnated by nitrate salts of nickel and iron and carbonized at 973 K. After this step, the nickel was in an elemental state, while the iron was in a magnetite form in the corresponding supports. Then, Pd and Pt particles were deposited onto the supports and the catalyst surface; precious metal nanoparticles (10-20 nm) were clustered inside spherical aggregated particles 500-600 nm in size. The final bimetallic catalysts (i.e., Pd-Pt/CCB, Pd-Pt/Ni-CCB, and Pd-Pt/FeO-CCB) were tested in hydrogenation of chlorate ions in the aqueous phase. For the nickel-promoted Pd-Pt catalyst, a >99% chlorate conversion was reached after 45 min at 80 °C. In contrast, the magnetite-promoted sample reached an 84.6% chlorate conversion after 3 h. Reuse tests were also carried out with the catalysts, and in the case of Pd-Pt/Ni-CCB after five cycles, the catalytic activity only decreased by ~7% which proves the stability of the system.

摘要

纤维素颗粒经过碳化处理后,被用作镍和磁铁矿促进的双金属钯和铂载体制备催化剂。双金属球形钯和铂颗粒的形成是为了增强贵金属在催化过程中的协同效应。首先,将基于纤维素珠的载体用镍和铁的硝酸盐浸渍并在 973 K 下碳化。在此步骤之后,镍处于元素态,而铁则以磁铁矿的形式存在于相应的载体中。然后,将钯和铂颗粒沉积到载体和催化剂表面上;贵金属纳米颗粒(10-20nm)在大小为 500-600nm 的球形聚集颗粒内团聚。最终的双金属催化剂(即 Pd-Pt/CCB、Pd-Pt/Ni-CCB 和 Pd-Pt/FeO-CCB)在水相中氯酸盐离子的加氢反应中进行了测试。对于镍促进的 Pd-Pt 催化剂,在 80°C 下反应 45 分钟后,氯酸盐的转化率超过 99%。相比之下,磁铁矿促进的样品在 3 小时后达到 84.6%的氯酸盐转化率。还对催化剂进行了重复使用测试,对于 Pd-Pt/Ni-CCB,在五个循环后,催化活性仅下降了约 7%,这证明了该系统的稳定性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/11ee/8584269/1186a5099297/ijms-22-11846-g001.jpg

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