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275 results on '"Lu, Ji-Qing"'

15. Selective Increase in CO2 Electroreduction to Ethanol Activity at Nanograin‐Boundary‐Rich Mixed Cu(I)/Cu(0) Sites via Enriching Co‐Adsorbed CO and Hydroxyl Species.

Author

Zhang, Ting, Xu, Shenglin, Chen, De‐Li, Luo, Ting, Zhou, Jinlei, Kong, Lichun, Feng, JiuJu, Lu, Ji‐Qing, Weng, Xuexiang, Wang, Ai‐Jun, Li, Zhengquan, Su, Yaqiong, and Yang, Fa

Subjects
ELECTROCHEMICAL analysis, COPPER surfaces, STANDARD hydrogen electrode, COPPER, RADIOLABELING
Abstract

Selective producing ethanol from CO2 electroreduction is highly demanded, yet the competing ethylene generation route is commonly more thermodynamically preferred. Herein, we reported an efficient CO2‐to‐ethanol conversion (53.5 % faradaic efficiency at −0.75 V versus reversible hydrogen electrode (vs. RHE)) over an oxide‐derived nanocubic catalyst featured with abundant "embossment‐like" structured grain‐boundaries. The catalyst also attains a 23.2 % energy efficiency to ethanol within a flow cell reactor. In situ spectroscopy and electrochemical analysis identified that these dualphase Cu(I) and Cu(0) sites stabilized by grain‐boundaries are very robust over the operating potential window, which maintains a high concentration of co‐adsorbed *CO and hydroxyl (*OH) species. Theoretical calculations revealed that the presence of *OHad not only promote the easier dimerization of *CO to form *OCCO (ΔG~0.20 eV) at low overpotentials but also preferentially favor the key *CHCOH intermediate hydrogenation to *CHCHOH (ethanol pathway) while suppressing its dehydration to *CCH (ethylene pathway), which is believed to determine the remarkable ethanol selectivity. Such imperative intermediates associated with the bifurcation pathway were directly distinguished by isotope labelling in situ infrared spectroscopy. Our work promotes the understanding of bifurcating mechanism of CO2ER‐to‐hydrocarbons more deeply, providing a feasible strategy for the design of efficient ethanol‐targeted catalysts. [ABSTRACT FROM AUTHOR]

Published
2024
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32. Acidic CO2 Electrolysis Addressing the "Alkalinity Issue" and Achieving High CO2 Utilization.

Author

Zhang, Ting, Zhou, Jinlei, Luo, Ting, Lu, Ji‐Qing, Li, Zhengquan, Weng, Xuexiang, and Yang, Fa

Subjects
ELECTROLYSIS, HYDROGEN evolution reactions, ELECTROLYTIC reduction, ALKALINITY, CARBON offsetting, DIRECT methanol fuel cells, STRUCTURAL design
Abstract

Electrochemical CO2 reduction reaction (CO2RR) provides a promising approach for sustainable chemical fuel production of carbon neutrality. Neutral and alkaline electrolytes are predominantly employed in the current electrolysis system, but with striking drawbacks of (bi)carbonate (CO32−/HCO3−) formation and crossover due to the rapid and thermodynamically favourable reaction between hydroxide (OH−) with CO2, resulting in low carbon utilization efficiency and short‐lived catalysis. Very recently, CO2RR in acidic media can effectively address the (bi)carbonate issue; however, the competing hydrogen evolution reaction (HER) is more kinetically favourable in acidic electrolytes, which dramatically reduces CO2 conversion efficiency. Thus, it is a big challenge to effectively suppress HER and accelerate acidic CO2RR. In this review, we begin by summarizing the recent progress of acidic CO2 electrolysis, discussing the key factors limiting the application of acidic electrolytes. We then systematically discuss addressing strategies for acidic CO2 electrolysis, including electrolyte microenvironment modulation, alkali cations adjusting, surface/interface functionalization, nanoconfinement structural design, and novel electrolyzer exploitation. Finally, the new challenges and perspectives of acidic CO2 electrolysis are suggested. We believe this timely review can arouse researchers′ attention to CO2 crossover, inspire new insights to solve the "alkalinity problem" and enable CO2RR as a more sustainable technology. [ABSTRACT FROM AUTHOR]

Published
2023
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