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Ag _x Cu _y Ni _z Trimetallic Alloy Catalysts for the Electrocatalytic Reduction of Benzyl Bromide in the Presence of Carbon Dioxide.

ABSTRACT: Different compositions of trimetallic alloy containing silver, copper, and nickel (Ag _x Cu _y Ni _z ) were electrodecorated in a protic ionic liquid medium on glassy carbon electrodes in order to investigate the suitability of the materials as catalysts for electrochemical reduction of carbon dioxide (CO₂). Surface characteristic morphology obtained by scanning electron microscopy shows cauliflower crystallites for the deposit of Ag, whereas materials of Cu and Ni exhibit cubic grains and fine particles, respectively. Deposits of trimetallic alloy containing Ag, Cu, and Ni exhibit the mixture of the three characteristic features. Further, trimetallic alloy containing a large amount of Ag provides high crystallinity, whereas predominance of Cu as well as Ni results in porous structures, as revealed by X-ray diffraction analysis. Atomic absorption spectroscopy () was used to determine the compositions of different alloy materials. The suitability of nanomaterials as cathodes for electroreduction of benzyl bromide in CO₂ containing 0.1 M tetra-n-butylammonium tetrafluoroborate (DMF/TBABF₄)/N,N-dimethylformamide medium was explored. The linear sweep voltammogram reveals that Ag₄₆Cu₄₀Ni₁₄ shows higher cathodic peak current and lower cathodic peak potential than those of other deposited nanomaterials as well as alloys, indicating its higher catalytic activity for such an electroreduction process, whereas potentiostatic electrolysis confirms the abovementioned results.

SUBMITTER: Rajagopal V

PROVIDER: S-EPMC6643392 | biostudies-literature | 2018 Dec

REPOSITORIES: biostudies-literature

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Ag x Cu y Ni z Trimetallic Alloy Catalysts for the Electrocatalytic Reduction of Benzyl Bromide in the Presence of Carbon Dioxide.

Rajagopal Venkatachalam V Manivel Perumal P Nesakumar Noel N Kathiresan Murugavel M Velayutham David D Suryanarayanan Vembu V

ACS omega 20181212 12

Different compositions of trimetallic alloy containing silver, copper, and nickel (Ag x Cu y Ni z ) were electrodecorated in a protic ionic liquid medium on glassy carbon electrodes in order to investigate the suitability of the materials as catalysts for electrochemical reduction of carbon dioxide (CO2). Surface characteristic morphology obtained by scanning electron microscopy shows cauliflower crystallites for the deposit of Ag, ...[more]

PMID: 31458333

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Project description:A composition spread alloy film (CSAF) spanning all of AgxPd1-x composition space, xPd = 0 → 1, was used to study catalytic ethylene hydrogenation with and without the presence of O2 in the feed gas. High-throughput measurements of the ethylene hydrogenation activity of AgxPd1-x alloys were performed at 100 Pd compositions spanning xPd = 0 → 1. The extent of ethylene hydrogenation was measured versus xPd at reaction temperatures spanning T = 300 → 405 K and inlet hydrogen partial pressures spanning PH2in = 70 → 690 Torr. The inlet ethylene partial pressure was constant at PC2H4in = 25 Torr, and the O2 inlet partial pressure was either PO2in = 0 or 15 Torr. When PO2in = 0 Torr, only those alloys with xPd ≥ 0.90 displayed observable ethylene hydrogenation activity. As expected, the most active catalyst was pure Pd, which yielded a maximum conversion of ∼0.4 at T = 405 K and PH2in = 690 Torr. Adding a constant O2 partial pressure of PO2in = 15 Torr to the feed stream dramatically increased the catalytic activity across the CSAF at all experimental conditions and catalyst compositions without inducing catalytic ethylene combustion and without measurable O2 consumption. The presence of PO2in = 15 Torr more than doubled the maximum achievable conversion on Pd to ∼0.9 and activated alloys with as little as xPd = 0.6 for ethylene hydrogenation. Measurement of the reaction order with respect to hydrogen, nH2, showed that nH2 ≈ 0 when PO2in = 15 Torr on high xPd alloys but that nH2 increases to values between 0.5 and 1 as xPd decreases or when PO2in = 0 Torr. We attribute this PO2in-induced change in nH2 to a change in the reaction mechanism resulting from different functional catalyst surfaces: one that is O2-activated and Pd-rich and one that is Ag-capped with low activity. Both are extremely sensitive to the bulk alloy composition, xPd, and the reaction temperature, T. These results show that the activity of AgPd catalysts for ethylene hydrogenation depends strongly on the operational conditions. Furthermore, we demonstrate that the exposure of AgPd catalysts to 15 Torr of O2 at moderate temperatures leads to enhanced catalyst performance, presumably by stimulating both Pd segregation to the topmost surface and Pd activation for ethylene hydrogenation.

Dataset Information

Ag _x Cu _y Ni _z Trimetallic Alloy Catalysts for the Electrocatalytic Reduction of Benzyl Bromide in the Presence of Carbon Dioxide.

Publications

Ag <sub><i>x</i></sub> Cu <sub><i>y</i></sub> Ni <sub><i>z</i></sub> Trimetallic Alloy Catalysts for the Electrocatalytic Reduction of Benzyl Bromide in the Presence of Carbon Dioxide.

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