Sulfur-doped unsaturated Ni-N3 coordination for efficient electroreduction of CO2

Yáng, Xiàn; Cheng, Jun; Lv, Hongkun; Yang, Xiao Qing; Ding, Liwei; Yang, Xu; Zhang, Kang; Sun, Wenjuan; Zhou, Junhu

doi:10.1016/j.cej.2022.137950

Cited by 45 publications

(31 citation statements)

References 42 publications

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“…Based on the above analysis, we can conclude that the in situ introduction of MA into ZIF-8 can apparently increase the Ni loading and prevent the Ni agglomeration by increasing the external surface areas of ZIF-8 (more Ni doping sites) and enhancing the anchoring effect of N coordination (lower Ni mobility). As a result, we obtain a Ni@NNC SACS with a high Ni single-atom content of 3.3 wt %, which is one of the highest values among all Ni-doped ZIF-8-derived single-atom catalysts, as seen in Figure S4. ,,− We therefore expect that Ni@NNC should show superior electrochemical catalysis performance as a separator modifier in the Li–S batteries.…”

Section: Resultsmentioning

confidence: 83%

In Situ Trapping Strategy Enables a High-Loading Ni Single-Atom Catalyst as a Separator Modifier for a High-Performance Li–S Battery

Sun

Chen

et al. 2023

ACS Appl. Mater. Interfaces

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The poor electrochemical reaction kinetics of Li polysulfides is a key barrier that prevents the Li−S batteries from widespread applications. Ni single atoms dispersed on carbon matrixes derived from ZIF-8 are a promising type of catalyst for accelerating the conversion of active sulfur species. However, Ni favors a square-planar coordination that can only be doped on the external surface of ZIF-8, leading to a low loading amount of Ni single atoms after pyrolysis. Herein, we demonstrate an in situ trapping strategy to synthesize Ni and melamine-codoped ZIF-8 precursor (Ni-ZIF-8-MA) by simultaneously introducing melamine and Ni during the synthesis of ZIF-8, which can remarkably decrease the particle size of ZIF-8 and further anchor Ni via Ni−N 6 coordination. Consequently, a novel high-loading Ni single-atom (3.3 wt %) catalyst implanted in an N-doped nanocarbon matrix (Ni@NNC) is obtained after high-temperature pyrolysis. This catalyst as a separator modifier shows a superior catalytic effect on the electrochemical transitions of Li polysulfides, which endows the corresponding Li−S batteries with a high specific capacity of 1232.4 mA h g −1 at 0.3 C and an excellent rate capability of 814.9 mA h g −1 at 3 C. Furthermore, a superior areal capacity of 4.6 mA h cm −2 with stable cycling over 160 cycles can be achieved under a critical condition with a low electrolyte/sulfur ratio (8.4 μL mg −1 ) and high sulfur loading (4.85 mg cm −2 ). The outstanding electrochemical performances can be attributed to the strong adsorption and fast conversion of Li polysulfides on the highly dense active sites of Ni@NNC. This intriguing work provides new inspirations for designing high-loading single-atom catalysts applied in Li−S batteries.

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Section: Resultsmentioning

confidence: 83%

In Situ Trapping Strategy Enables a High-Loading Ni Single-Atom Catalyst as a Separator Modifier for a High-Performance Li–S Battery

Sun

Chen

et al. 2023

ACS Appl. Mater. Interfaces

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“…11 In addition, the hydrogen evolution reaction (HER) occurs frequently as a side reaction during CO 2 reduction, which decreases the selectivity for the ERCO 2 . 12,13 Therefore, it is crucial to develop a catalyst with high activity for the ERCO 2 and inhibition for the HER.…”

Section: Jiaying Yanmentioning

confidence: 99%

Structure-evolved YbBiO₃perovskites for highly formate-selective CO₂electroreduction

et al. 2023

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“…[32] Ni-SNC catalysts was prepared by calcining SO 4 2À doped Zn/Ni ZIF-8 with Zn(SO 4 ) 2 as the sulfur source. [33] A Higher loadings of metal monatomic catalysts and higher doping ratios may be obtained using the impregnation approach, allowing the electrocatalysts to be optimized for activity and selectivity towards ECR. [34]…”

Section: Impregnationmentioning

confidence: 99%

“…From the perspective of reaction process, (1) the modulation of the electronic structure of the central metal has a huge effect on the adsorption and desorption behaviors of the intermediates generated in the ECR process. Such as the adsorption intensity of *COOH, [25,[32][33]38,[48][49]54,56,[60][61]69,71] *OCHO [55,59] and *COH, [58] thus influence the selectivity for various products formed in ECR process; (2) the doping of heteroatom like S in Fe-N-C, modified electronic structure of the metal center can hasten the dissociation of H 2 O into *H, [39,51,63] accelerating the first step of the electron-proton coupling process in the ECR for the production of CO, thus increase the selectivity of the prepared M-SACs for CO generation.…”

Section: Conclusion and Challengesmentioning

confidence: 99%

“…Moreover, in a planar structure like graphene, it is proposed that edge-anchored unsaturated NiN 2 (NH 2 ) and NiN 3 sites may be the effective active sites for the conversion CO 2 to CO. For Ni single-atom catalyst with both S doping and unsaturated Ni-N 3 coordination, the redistribution of electron structure of Ni center reduces the energy barrier for the formation of *COOH and reduces the adsorption energy of *CO, facilitating the production of CO during ECR process. [33] Heteroatom doped asymmetric Cu-N x -C SACs Currently, copper is the only transition metal catalyst that can efficiently generate C 2 + products due to the specific binding energy of the *CO intermediates, great efforts have been paid to study Cu based catalysts. However, only C 1 product can be formed for SACs with Cu-N 4 site due to the lack of CÀ C coupling site.…”

Section: Heteroatom Doped Asymmetric Ni-n X -C Sacsmentioning

confidence: 99%

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Heteroatom‐Doped Asymmetric Metal‐N_x‐C Single Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Kong

Wang

Jiang

2022

Chemistry An Asian Journal

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CO 2 utilization is one of the hottest research topics worldwide. As a class of newly emerging and promising catalysts for electrochemical CO 2 reduction (ECR) reaction, heteroatom-doped metal-N x -C single atom catalysts (M-N x -C SACs) attract extensive attentions. Nowadays, great progress, including structure modulation, identification of local coordination environment and ECR mechanism via advanced synthetic strategies, characterization techniques and theoretical calculations, have been achieved over heteroatom doped asymmetric M-N x -C SACs, which boost the ECR performances and deepen the understanding of ECR mechanism. In this context, we summarize recent progresses in heteroatomdoped asymmetric M-N x -C SACs, with emphasis on synthetic strategies and their applications in ECR reaction, along with current understanding on the ECR mechanisms both experimentally and theoretically. Finally, the challenges and perspectives for the heteroatom-doped asymmetric M-N x -C SACs towards ECR are proposed.

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Sulfur-doped unsaturated Ni-N3 coordination for efficient electroreduction of CO2

Cited by 45 publications

References 42 publications

In Situ Trapping Strategy Enables a High-Loading Ni Single-Atom Catalyst as a Separator Modifier for a High-Performance Li–S Battery

In Situ Trapping Strategy Enables a High-Loading Ni Single-Atom Catalyst as a Separator Modifier for a High-Performance Li–S Battery

Structure-evolved YbBiO₃perovskites for highly formate-selective CO₂electroreduction

Heteroatom‐Doped Asymmetric Metal‐N_x‐C Single Atom Catalysts for Electrochemical CO₂ Reduction Reaction

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Sulfur-doped unsaturated Ni-N3 coordination for efficient electroreduction of CO2

Cited by 45 publications

References 42 publications

In Situ Trapping Strategy Enables a High-Loading Ni Single-Atom Catalyst as a Separator Modifier for a High-Performance Li–S Battery

In Situ Trapping Strategy Enables a High-Loading Ni Single-Atom Catalyst as a Separator Modifier for a High-Performance Li–S Battery

Structure-evolved YbBiO3perovskites for highly formate-selective CO2electroreduction

Heteroatom‐Doped Asymmetric Metal‐Nx‐C Single Atom Catalysts for Electrochemical CO2 Reduction Reaction

Contact Info

Product

Resources

About

Structure-evolved YbBiO₃perovskites for highly formate-selective CO₂electroreduction

Heteroatom‐Doped Asymmetric Metal‐N_x‐C Single Atom Catalysts for Electrochemical CO₂ Reduction Reaction