Journal
ACS CATALYSIS
Volume 12, Issue 9, Pages 4840-4847Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c00430
Keywords
electrochemical semihydrogenation; interfacial water; Raman spectroscopy; Fe doping; alkynes
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Funding
- Natural Science Foundation of China [51902077, 21725102, 91961106]
- Zhejiang Provincial Natural Science Foundation [LQ19B010001]
- Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang [2020R01002]
- general items of Zhejiang Provincial Department of Education [Y201840068]
- Zhejiang Province Ten Thousand People Plan
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By designing the catalyst based on the interfacial water structure, this study achieved high activity and selectivity in electrochemical semihydrogenation. Experimental results showed that PdFe nanosheets could continuously produce a large amount of alkynes for 264 hours, demonstrating significant advantages over traditional thermal semihydrogenation methods in terms of performance, energy, and cost.
Electrochemical semihydrogenation (ECSH) of alkynes to alkenes is an ideal alternative to traditional thermal semihydrogenation, and yet is limited by low conversion yield and product selectivity. Here, we offer an insight into the catalyst design from the viewpoint of an interfacial water structure toward highly active and selective ECSH. In situ Raman spectroscopy measurements combined with theoretical calculations reveal that the structure of interfacial water on Pd nanosheets can be altered by Fe doping toward trihedrally coordinated water and dangling O-H water, which in turn boosts the activity and selectivity in ECSH. Remarkably, the PdFe nanosheets can sustain continuous 264 h of electrolysis with 100-fold amplified amount of alkynes production in a flow cell. We also demonstrate the incomparable superiority for ECSH of alkynes to alkenes in terms of performance, energy, and cost.
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