Mahajan Ankita, Banik Senjuti, Majumdar Dipanwita, Bhattacharya Swapan Kumar
Physical Chemistry Section, Department of Chemistry, Jadavpur University, Kolkata, 700 032 West Bengal, India.
Department of Chemistry, Chandernagore College, Chandannagar, Hooghly, 712136 West Bengal, India.
ACS Omega. 2019 Mar 4;4(3):4658-4670. doi: 10.1021/acsomega.8b03561. eCollection 2019 Mar 31.
Reduced graphene oxide (RGO)-supported bimetallic Pd Ag alloy nanoparticles of various compositions were synthesized by one-pot coreduction of respective precursors with hydrazine for use in the anode catalysis of oxidation of butan-1-ol in alkali. The as-synthesized catalyst materials were characterized by microscopic, spectroscopic, and diffraction techniques. Cyclic voltammetry (CV), chronoamperometry, and polarization studies infer that a few Pd Ag materials exhibit an enhanced and synergistic catalytic activity in reference to Pd and Ag nanomaterials. Among the various RGO composites of Pd Ag alloy on graphite support, the one containing the PdAg@RGO composite is the best in catalytic activity. The cycle life of the catalyst is found to be very high, and PdO and AgO are found to be generated in the catalyst material with little change in the catalytic capability during the 100th cycle of CV operation. The addition of Ag upto 30 atom % in the Pd Ag alloy causes greater formation of butyraldehyde and butyl butanoate among the various products. Larger atom % of Pd helps to form sodium butyrate and sodium carbonate, as evident from the ex situ Fourier transform infrared and high-performance liquid chromatography study of the product mixtures and the separate CV studies of the intermediate products. A suitable mechanism is also proposed to fit the findings.
通过用肼一锅共还原各自的前驱体，合成了具有不同组成的还原氧化石墨烯（RGO）负载的双金属Pd-Ag合金纳米颗粒，用于碱性条件下丁醇-1氧化的阳极催化。通过显微镜、光谱和衍射技术对合成的催化剂材料进行了表征。循环伏安法（CV）、计时电流法和极化研究表明，一些Pd-Ag材料相对于Pd和Ag纳米材料表现出增强的协同催化活性。在石墨载体上的各种Pd-Ag合金的RGO复合材料中，含有PdAg@RGO复合材料的催化活性最佳。发现催化剂的循环寿命非常高，并且在CV操作的第100个循环期间，催化剂材料中生成了PdO和AgO，催化能力几乎没有变化。在Pd-Ag合金中添加高达30原子%的Ag会导致各种产物中丁醛和丁酸丁酯的生成量增加。从产物混合物的非原位傅里叶变换红外光谱和高效液相色谱研究以及中间产物的单独CV研究可以看出，较大原子百分比的Pd有助于形成丁酸钠和碳酸钠。还提出了一个合适的机制来符合这些发现。
