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Engineering single-atomic Ni sites stabilized with adjacent spinel nanoparticles to boost CO2 electroreduction.

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Title: Engineering single-atomic Ni sites stabilized with adjacent spinel nanoparticles to boost CO2 electroreduction.
Authors: Ping, Dan1 (AUTHOR), Feng, Yichen1 (AUTHOR), Wu, Shide1 (AUTHOR) wushide@zzuli.edu.cn, Wang, Dingsheng2 (AUTHOR), Liu, Weitao1 (AUTHOR), Zhang, Qikang1 (AUTHOR), Fang, Hua3 (AUTHOR), Li, Yanyan1 (AUTHOR), Liu, Bingkun1 (AUTHOR), Zhang, Jianqiang1 (AUTHOR), Wang, Shiwen3 (AUTHOR), Fang, Shaoming1 (AUTHOR) mingfang@zzuli.edu.cn
Source: Separation & Purification Technology. May2025:Part B, Vol. 357, pN.PAG-N.PAG. 1p.
Subjects: Oxygen vacancy, Chemical kinetics, Carbon dioxide, Atoms, Spinel
Abstract: [Display omitted] • A single-atomic Ni catalyst stabilized by MgAl 2 O 4 nanoparticles is developed via a facile pyrolysis strategy. • The NiMgAl LDHs self-confinement metal precursor and its derived MgAl 2 O 4 are crucial for stabilizing Ni atoms. • High selectivity with CO Faradaic efficiency nearly 100% and remarkable stability are demonstrated. • Unveiling the indispensible role of MgAl 2 O 4 in boosting CO 2 RR and suppressing HER. Single-atom catalysts show great potential in the electrochemical CO 2 reduction reaction (CO 2 RR), but face significant challenges in accelerating reaction kinetics. Herein, we develop a three-dimensional heterostructured MgAl 2 O 4 /Ni-N-C catalyst via a facile pyrolysis strategy, featuring abundant atomically dispersed Ni sites and ∼14 nm MgAl 2 O 4 nanoparticles. The MgAl 2 O 4 with rich oxygen vacancies is crucial for stabilizing Ni atoms and promoting CO 2 activation, thereby contributing to an excellent selectivity of nearly 100 % and good stability for CO production. The CO Faraday efficiency remains > 90 % within a large potential window (−0.57 to −0.97 V vs. RHE), and achieves the maximum of 98.7 % at −0.82 V. Theoretical calculations reveal that MgAl 2 O 4 introduction can modulate the electron structure of Ni atoms, and accelerate the formation of *COOH intermediate, thus boosting CO 2 RR performance. This research provides a novel approach for the design of high-efficiency single-atom catalysts for CO 2 conversion. [ABSTRACT FROM AUTHOR]
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Database: Engineering Source
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Abstract:[Display omitted] • A single-atomic Ni catalyst stabilized by MgAl 2 O 4 nanoparticles is developed via a facile pyrolysis strategy. • The NiMgAl LDHs self-confinement metal precursor and its derived MgAl 2 O 4 are crucial for stabilizing Ni atoms. • High selectivity with CO Faradaic efficiency nearly 100% and remarkable stability are demonstrated. • Unveiling the indispensible role of MgAl 2 O 4 in boosting CO 2 RR and suppressing HER. Single-atom catalysts show great potential in the electrochemical CO 2 reduction reaction (CO 2 RR), but face significant challenges in accelerating reaction kinetics. Herein, we develop a three-dimensional heterostructured MgAl 2 O 4 /Ni-N-C catalyst via a facile pyrolysis strategy, featuring abundant atomically dispersed Ni sites and ∼14 nm MgAl 2 O 4 nanoparticles. The MgAl 2 O 4 with rich oxygen vacancies is crucial for stabilizing Ni atoms and promoting CO 2 activation, thereby contributing to an excellent selectivity of nearly 100 % and good stability for CO production. The CO Faraday efficiency remains > 90 % within a large potential window (−0.57 to −0.97 V vs. RHE), and achieves the maximum of 98.7 % at −0.82 V. Theoretical calculations reveal that MgAl 2 O 4 introduction can modulate the electron structure of Ni atoms, and accelerate the formation of *COOH intermediate, thus boosting CO 2 RR performance. This research provides a novel approach for the design of high-efficiency single-atom catalysts for CO 2 conversion. [ABSTRACT FROM AUTHOR]
ISSN:13835866
DOI:10.1016/j.seppur.2024.130193