Ni and nitrogen-codoped ultrathin carbon nanosheets with strong bonding sites for efficient CO2 electrochemical reduction

Ma, Zhongjun; Zhang, Xilin; Wu, Dapeng; Han, Xueyun; Zhang, Lumin; Wang, Hongju; Xu, Fang; Gao, Zhiyong; Jiang, Kai

doi:10.1016/j.jcis.2020.02.050

Cited by 37 publications

(21 citation statements)

References 59 publications

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“…Ni atoms can combine with three or four nitrogen atoms, and the environment of center metal atoms greatly influences CO 2 RR. Wang et al and Li et al study the reaction energy and the intermediates of the structure that is Ni with different combinations of carbon and nitrogen atoms and find that the energy barrier of the intermediate Ã COOH (the key intermediate of CO 2 R) increase with more nitrogen atoms combines with Ni, but the desorption of CO become much more accessible [27,28]. Zhao et al used the solvation model to study nickel catalysts with different coordination further.…”

mentioning

confidence: 99%

Reaction mechanism on Ni-C₂-NS single-atom catalysis for the efficient CO₂reduction reaction

Yuan

et al. 2021

Journal of Experimental Nanoscience

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Ni-based single-atom catalysis (Ni-SAC) has been experimentally reported with superior performance in reducing CO 2 to CO. However, due to the ambiguities in its structures, the active sites of Ni-SAC that are responsible for superior performance have not yet been resolved. This work investigates the CO 2 reduction reaction (CO 2 RR) mechanism on Ni-SAC by carrying out quantum mechanics (QM) simulation to consider both solvation effects. After exploring multiple possible combinations of N, S, and C, we distinguish a Ni-SAC site with two C, one S, and one N, representing the best performance. The predicted formation energy is closely consistent with experimental onset potential. Our prediction also suggests further improvement by finely tuning the electronics state of metal sites by changing the SAC support.

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confidence: 99%

Reaction mechanism on Ni-C₂-NS single-atom catalysis for the efficient CO₂reduction reaction

Yuan

et al. 2021

Journal of Experimental Nanoscience

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“…The methodology resulted in a simple and rapid construction of catalysts with single atoms avoiding their aggregation, originating active Ni-N sites that allowed the reduction of CO 2 to CO with a faradic efficiency equal to 90.2% and an overpotential of 0.69 V vs. RHE. Ma and co-workers [152] were able to synthesize an inexpensive carbon matrix with easily available components such as melanin and citric acid, which after a pyrolysis process, obtain ultra-thin nano-sheets doped with single Ni atoms. Yang and co-workers [153] proposed a scalable strategy to obtain catalysts with single Cu atoms.…”

Section: Smas-n-other Carbon Materialsmentioning

confidence: 99%

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

et al. 2021

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The global warming and the dangerous climate change arising from the massive emission of CO2 from the burning of fossil fuels have motivated the search for alternative clean and sustainable energy sources. However, the industrial development and population necessities make the decoupling of economic growth from fossil fuels unimaginable and, consequently, the capture and conversion of CO2 to fuels seems to be, nowadays, one of the most promising and attractive solutions in a world with high energy demand. In this respect, the electrochemical CO2 conversion using renewable electricity provides a promising solution. However, faradaic efficiency of common electro-catalysts is low, and therefore, the design of highly selective, energy-efficient, and cost-effective electrocatalysts is critical. Carbon-based materials present some advantages such as relatively low cost and renewability, excellent electrical conductivity, and tunable textural and chemical surface, which show them as competitive materials for the electro-reduction of CO2. In this review, an overview of the recent progress of carbon-based electro-catalysts in the conversion of CO2 to valuable products is presented, focusing on the role of the different carbon properties, which provides a useful understanding for the materials design progress in this field. Development opportunities and challenges in the field are also summarized.

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“…Since the experimental results have proved the existing various M-N x (x = 1-4) sites after the catalyst preparation process, these sites were considered as possible active sites in mechanism studies. 37,66,70,71,75,82,83 The free energy change of the intermediates formed on M-N x sites was widely utilized to guide the mechanism study. For example, Zhao et al calculated the free energy change on four types of Ni-N x (x = 1-4) sites as shown in Figure 9.…”

Section: Reaction Mechanism and Active Sites Of M-sacs For Co 2 Rrmentioning

confidence: 99%

“…As discussed above, the coordination environment crucially impacts the electronic structure of metal center and determines the catalytic performance. Since the experimental results have proved the existing various M‐N x (x = 1–4) sites after the catalyst preparation process, these sites were considered as possible active sites in mechanism studies 37,66,70,71,75,82,83 …”

Section: M‐sacs For Co2rrmentioning

confidence: 99%

Recent progress in electrochemical reduction of carbon dioxide on metal single‐atom catalysts

Huo

Wang

2021

Energy Science & Engineering

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Electrochemical reduction reaction of CO2 (CO2RR) is a promising technology for alleviating the global warming caused by the emission of CO2. This technology, however, is still in the stage of finding efficient catalysts. The catalysts must be able to convert CO2 to other carbon‐based products with high activity and selectivity to valuable chemicals. In this review, previous development of heteroatom‐doped metal‐free carbon materials (H‐CMs) is briefly summarized. Recent progress of CO2RR promoted by metal single‐atom catalysts (M‐SACs) is then discussed with emphasis on the synthesis of M‐SACs, the catalytic performance, and reaction mechanisms. The high temperature pyrolysis method and electrodeposition are attracting attentions recently to prepare M‐SACs with high metal loading on N‐doped carbon materials, a very active M‐SACs system for the CO2RR. Theoretical calculations of free energy change on active sites, the Operando X‐ray absorption near edge structure (XANES), and Bader charge analysis reveal a significant role of metal oxidation state and charge transfer between metal atoms and absorbed CO. The challenges and perspectives for the extensive applications of M‐SACs in CO2RR are also discussed in this review.

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Ni and nitrogen-codoped ultrathin carbon nanosheets with strong bonding sites for efficient CO2 electrochemical reduction

Cited by 37 publications

References 59 publications

Reaction mechanism on Ni-C₂-NS single-atom catalysis for the efficient CO₂reduction reaction

Reaction mechanism on Ni-C₂-NS single-atom catalysis for the efficient CO₂reduction reaction

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

Recent progress in electrochemical reduction of carbon dioxide on metal single‐atom catalysts

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Ni and nitrogen-codoped ultrathin carbon nanosheets with strong bonding sites for efficient CO2 electrochemical reduction

Cited by 37 publications

References 59 publications

Reaction mechanism on Ni-C2-NS single-atom catalysis for the efficient CO2reduction reaction

Reaction mechanism on Ni-C2-NS single-atom catalysis for the efficient CO2reduction reaction

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

Recent progress in electrochemical reduction of carbon dioxide on metal single‐atom catalysts

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Reaction mechanism on Ni-C₂-NS single-atom catalysis for the efficient CO₂reduction reaction

Reaction mechanism on Ni-C₂-NS single-atom catalysis for the efficient CO₂reduction reaction