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    董盛红, 陈金铸, 郭旭虹, 徐益升. 可见光诱导Pd-Pt/RGO-g-C3N4催化苯甲醛选择性加氢[J]. 华东理工大学学报(自然科学版), 2019, 45(3): 365-373. DOI: 10.14135/j.cnki.1006-3080.20180426001
    引用本文: 董盛红, 陈金铸, 郭旭虹, 徐益升. 可见光诱导Pd-Pt/RGO-g-C3N4催化苯甲醛选择性加氢[J]. 华东理工大学学报(自然科学版), 2019, 45(3): 365-373. DOI: 10.14135/j.cnki.1006-3080.20180426001
    DONG Shenghong, CHEN Jinzhu, GUO Xuhong, XU Yisheng. RGO-g-C3N4 Supported Palladium-Platinum Alloy for Selective Hydrogenation of Benzaldehyde under Visible-Light Irradiation[J]. Journal of East China University of Science and Technology, 2019, 45(3): 365-373. DOI: 10.14135/j.cnki.1006-3080.20180426001
    Citation: DONG Shenghong, CHEN Jinzhu, GUO Xuhong, XU Yisheng. RGO-g-C3N4 Supported Palladium-Platinum Alloy for Selective Hydrogenation of Benzaldehyde under Visible-Light Irradiation[J]. Journal of East China University of Science and Technology, 2019, 45(3): 365-373. DOI: 10.14135/j.cnki.1006-3080.20180426001

    可见光诱导Pd-Pt/RGO-g-C3N4催化苯甲醛选择性加氢

    RGO-g-C3N4 Supported Palladium-Platinum Alloy for Selective Hydrogenation of Benzaldehyde under Visible-Light Irradiation

    • 摘要: 构建了还原氧化石墨烯(RGO)掺杂的石墨相碳化氮载体(RGO-g-C3N4),制备了负载型双金属Pd-Pt/RGO-g-C3N4催化剂,通过高分辨透射电镜(HRTEM)、X射线光电子能谱(XPS)、X射线粉末衍射(XRD)、氮吸附-脱附和电感耦合等离子发射光谱(ICP)等手段对催化剂进行了系统表征,并成功将其应用于光催化苯甲醛的选择性加氢反应。考察了RGO的掺杂量、载体的掺杂类型、负载型金属种类等对该催化剂催化性能的影响。实验结果表明:当RGO掺杂量为1%(质量分数),Pd-Pt(nPdnPt=1∶1)合金负载量为3%(质量分数)时对反应的选择性最高,催化效果最好,苯甲醛催化加氢制备苯甲醇的收率高达81%。研究证实了负载型Pd-Pt/RGO-g-C3N4催化剂可以成功实现醛的光催化选择性加氢制醇,并有效克服传统的光催化反应效率低等问题。

       

      Abstract: A reduced graphene oxide (RGO)-doped graphite-phase carbon nitride (RGO-g-C3N4) was prepared, and then the Pd-Pt alloy nanoparticles were uniformly immobilized on the RGO-g-C3N4 (Pd-Pt/RGO-g-C3N4), giving rise to supported catalyst. The catalyst was characterized by high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), X-ray powder diffraction (XRD), nitrogen adsorption-desorption, and inductively coupled plasma atomic emission spectroscopy (ICP-AES). The obtained catalyst was then applied to catalyze the selective hydrogenation of benzaldehyde under the irradiation of visible-light. The XRD and the XPS analyses show that small amount doping of RGO or other additives do not change the structure of g-C3N4, and the nitrogen adsorption-desorption measurement indicates that small amount doping increases the specific surface area of the support. The HRTEM and the XPS analyses revealed that the noble metals on the support were successfully reduced by the NaBH4, and the resulting Pd-Pt alloy nanoparticles (NPs) showed a uniform size and were homogeneously distributed on the support. The optimal catalytic conditions for the reaction were investigated by changing the doping amount of RGO, the doping types on the supports including cobalt phthalocyanine and copper phthalocyanine, and the types of immobilized noble metals. The experimental results show that w=1% RGO doping with w=3% Pd-Pt (nPdnPt = 1∶1) alloy catalyst has the highest selectivity on the reaction, and the yield of benzyl alcohol is up to 81%. The results also demonstrate that Pd is the active sites of the Pd-Pt/RGO-g-C3N4 catalyst for the selective hydrogenation of benzaldehyde. The loading of Pt enhanced selectivity of the bimetallic Pd-Pt/RGO-g-C3N4. The study performed in this work shows that the supported Pd-Pt/RGO-g-C3N4 catalyst addresses the traditional problems of low photocatalytic efficiency, and successfully realizes the highly selective conversion of aldehyde into alcohol molecules.

       

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