Institution: | 1. Interdisciplinary Research Center for Hydrogen Technologies and Carbon Management, King Fahd University of Petroleum & Minerals (KFUPM), Dhahran, 31261 Saudi Arabia;2. School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300350 China.;3. Institute of Zhejiang University – Quzhou, Quzhou, 324000 China
Contribution: Investigation (supporting), Methodology (supporting);4. Interdisciplinary Research Center for Hydrogen Technologies and Carbon Management, King Fahd University of Petroleum & Minerals (KFUPM), Dhahran, 31261 Saudi Arabia
Contribution: Investigation (supporting), Resources (supporting), Validation (supporting);5. Department of Chemistry, TUM School of Natural Sciences, Technical University of Munich, Garching, 85748 Germany
Contribution: Investigation (supporting), Writing - review & editing (supporting);6. Department of Materials Science and Engineering, King Fahd University of Petroleum & Minerals, Dhahran, 31261 Saudi Arabia
Contribution: Investigation (supporting), Methodology (supporting);7. Chemical Engineering Department, King Fahd University of Petroleum & Minerals, Dhahran, 31261, Saudi Arabia
Contribution: Investigation (supporting), Methodology (supporting);8. State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China |
Abstract: | The practicality of the electrochemical CO2 reduction technique depends on the development of cost-effective, robust, and highly selective catalysts. To achieve this goal, we have engineered self-supported 3D electrodes composed of Pd-Zn nanosheets (NSs) for CO2 electrochemical reduction to CO with minimal Pd content. This innovative electrode with an increased surface area was created using an electrodeposition method employing a dynamic hydrogen bubble template. By precisely adjusting the Pd content, we improved the thickness, porosity, and surface area of the electrodes, resulting in a CO2-to-CO selectivity reaching as high as 88.5 %, with an average of at least 80 % sustained over 10 hours. This remarkable improved activity can be attributed to the synergistic effects of an appropriate Pd/Zn atomic ratio as well as to the large surface area of nanosheets structures with rich edge active sites. Furthermore, to get around the limitations of CO2 mass transfer, reactions were done at high pressures conditions ranging from 3 to 9.5 bar; this strategic approach yielded an outstanding partial current density of −304.6 mA cm−2 for CO. These noteworthy findings establish concepts for constructing effective and earth-abundant CO-producing electrocatalysts. |