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- W4386853732 abstract "One of the main research challenges for electrocatalysis that produces carbon-containing products from CO 2 is avoiding the competing hydrogen evolution reaction. Instead of totally eliminating hydrogen, our approach makes use of the readily available protons in aqueous electrolyte to co-produce CO and H 2 , making synthesis gas (syngas) with a tunable CO:H 2 ratio. The resulting syngas can then be used as feedstock for existing thermocatalytic processes, such as Fischer–Tropsch and methanol synthesis reactions [1]. We will present our results in identifying palladium hydride (PdH), formed under electrocatalytic reaction conditions, as an effective electrocatalyst that enables the syngas production [2]. We will also report our efforts in reducing the loading of Pd by alloying Pd with inexpensive secondary metals, supporting Pd on transition metal carbides and nitrides, and utilizing single atom Pd catalysts. For each type of the catalysts, we monitor the phase transition from Pd to PdH under reaction conditions with in-situ synchrotron-based X-ray absorption and X-ray diffraction techniques. We also identify descriptors for syngas production on PdH, bimetallic PdH, and supported PdH catalysts by performing DFT calculations of the effect of PdH formation on the binding strength of reaction intermediates. The research methodology established here should be useful not only for continued optimization of Pd-based syngas-producing electrocatalysts, but also for enhancing activity while reducing the loading of precious metals for other electrocatalytic applications. Furthermore, we will discuss our recent results in utilizing a tandem scheme of electrocatalytic-thermocatalytic processes to convert CO 2 to C 3 oxygenates [3]. [1] B.M. Tackett, E. Gomez and J.G. Chen, “Net reduction of CO 2 via its thermocatalytic and electrocatalytic transformation reactions in standard and hybrid processes”, Nature Catalysis , 2 (2019) 381. [2] B.M. Tackett, J.H. Lee and J.G. Chen, “Electrochemical Conversion of CO 2 to Syngas with Palladium-Based Electrocatalysts”, Accounts of Chemical Research , 53 (2020) 1535. [3] A.N. Biswas, Z. Xie, R. Xia, S. Overa, F. Jiao and J.G. Chen, “Tandem Electrocatalytic-Thermocatalytic Reaction Scheme for CO 2 Conversion to C 3 Oxygenates”, ACS Energy Letters , 7 (2022) 2904" @default.
- W4386853732 created "2023-09-20" @default.
- W4386853732 creator A5034358731 @default.
- W4386853732 date "2023-08-28" @default.
- W4386853732 modified "2023-09-27" @default.
- W4386853732 title "(Invited) Electrocatalytic Conversion of CO<sub>2</sub> to Syngas with Controlled CO/H<sub>2</sub> Ratios" @default.
- W4386853732 doi "https://doi.org/10.1149/ma2023-01372161mtgabs" @default.
- W4386853732 hasPublicationYear "2023" @default.
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