Dual atom catalysts for rapid electrochemical reduction of CO to ethylene

Journal Article · Fri Dec 01 00:00:00 EST 2023 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2023.108966· OSTI ID:2860500

Musgrave, Charles B.; Li, Yuyin; Luo, Zhengtang; Goddard, William A.

Strong CO adsorption and facile CO dimerization are the key challenges in electrochemical CO2 reduction towards multi-carbon (C2+) products. We recently showed that CoPc immobilized on a single-walled carbon nanotube can selectively reduce CO2 to methanol. This is enabled through molecular strain, which dramatically improves the CO adsorption energy to CoPc, which in turn facilitates methanol formation. We now examine the extended Phthalocyanine (PcEx) dual atom catalyst (DAC), which is intrinsically strained and contains two catalyst centers, making it a candidate for reducing CO to C2+ products. Using Quantum Mechanics (QM), we screened 20 elements embedded in the PcEx, seeking catalysts with weak hydrogen binding, strong CO binding, and facile CO dimerization. We identi>ied Fe, Ru, Co, and Ir as the best performers and subsequently evaluated the entire CO to C2H4 mechanism (9 steps) using each of these elements as catalysts. In terms of limiting potential and overall exergonicity, we identi>ied CoPcEx as the best catalyst, followed by IrPcEx. We then examined the full CO to C2H4 mechanism on the bimetallic IrCoPcEx catalyst using grand canonical QM to obtain the reaction energetics as a function of applied potential. We conclude that the bimetallic IrCoPcEx is most promising for ef>iciently converting CO to ethylene.

• Research Organization: California Institute of Technology
• Sponsoring Organization: Basic Energy Sciences; Office of Science; U.S. Department of Energy; USDOE Office of Science (SC), Basic Energy Sciences (BES)
• Grant/Contract Number: AC02-05CH11231; SC0021266
• Other Award/Contract Number: BES-ERCAP0024109
• OSTI ID: 2860500
• Alternate ID(s): OSTI ID: 2369940; OSTI ID: 2576922
• Journal Information: Nano Energy, Journal Name: Nano Energy Vol. 118; ISSN 2211-2855
• Publisher: Elsevier BV
• Country of Publication: United States
• Language: English