Bimetallic phthalocyanine heterostructure used for highly selective electrocatalytic CO2 reduction

Yang, Chenhuai; Gao, Zhonghui; Wang, Dingjia; Li, Shuyu; Li, Jun; Zhu, Yating; Wang, Haiqing; Yang, Wenjuan; Gao, Xuejiao J.; Zhang, Zhicheng; Hu, Wenping

doi:10.1007/s40843-021-1749-5

Cited by 44 publications

(13 citation statements)

References 65 publications

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“…11−17 However, as most of the obtained SACs have M (center metal)−N coordination, the tunability of the central metal atom electronic state is limited by pure N coordination. 18 Yu et al reported a Sn SAC named SnN 3 O 1 with three N atoms and one O atom coordinated with Sn in the first coordination shell. 19 This catalyst not only exhibited an excellent Faradaic efficiency of CO as high as 94% at −0.7 V vs RHE but also showed an outstanding turnover frequency (TOF) of up to 23340.5 h −1 .…”

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confidence: 99%

“…Recently, 3d carbon-supported transition-metal single-atom catalysts (SACs) have been extensively explored for the ECRR. − However, as most of the obtained SACs have M (center metal)–N coordination, the tunability of the central metal atom electronic state is limited by pure N coordination . Yu et al reported a Sn SAC named SnN 3 O 1 with three N atoms and one O atom coordinated with Sn in the first coordination shell .…”

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confidence: 99%

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Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction

Song

Zhao

et al. 2023

ACS Nano

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Cu single-atom catalysts (Cu SACs) have been considered as promising catalysts for efficient electrocatalytic CO 2 reduction reactions (ECRRs). However, the reports on Cu SACs with an asymmetric atomic interface to obtain CO are few. Herein, we rationally designed two Cu SACs with different asymmetric atomic interfaces to explore their catalytic performance. The catalyst of CuN 3 O/C delivers high ECRR selectivity with an FE CO value of above 90% in a wide potential window from −0.5 to −0.9 V vs RHE (in particular, 96% at −0.8 V), while CuCO 3 /C delivers poor selectivity for CO production with a maximum FE CO value of only 20.0% at −0.5 V vs RHE. Besides, CuN 3 O/C exhibited a large turnover frequency (TOF) up to 2782.6 h −1 at −0.9 V vs RHE, which is much better than the maximum 4.8 h −1 of CuCO 3 /C. Density functional theory (DFT) results demonstrate that the CuN 3 O site needs a lower Gibbs free energy than CuCO 3 in the rate-determining step of CO desorption, leading to the outstanding performance of CuN 3 O/C on the process of ECRR-to-CO. This work provides an efficient strategy to improve the selectivity and activity of the ECRR via regulating asymmetric atomic interfaces of SACs by adjusting the coordination atoms.

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confidence: 99%

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confidence: 99%

Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction

Song

Zhao

et al. 2023

ACS Nano

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“…The continuously excessive release of greenhouse gas, CO 2 , has caused serious global climate warming and environmental degradation. In this regard, the emerging sequestration [1], chemical fixation [2], and electro/photo/thermochemical reduction technologies [3][4][5][6][7][8][9] have been developed to alleviate CO 2 emissions. The electrochemical CO 2 reduction reaction (CO 2 RR) to yield high-value-added fuels and chemicals provides a promising approach towards an sustainable carbon-cycle utilization, especially when powered by renewable energy resources [10][11][12][13][14][15][16][17].…”

Section: Introductionmentioning

confidence: 99%

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Qiu

Wang

et al. 2022

Sci. China Mater.

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The electrochemical CO 2 reduction reaction (CO 2 RR) to yield high-value added fuels and chemicals provides a promising approach towards global carbon neutrality. Constant endeavors have been devoted to the exploration of high-efficiency catalyst with rapid reaction kinetics, low energy input, and high selectivity. In addition to the maximum metal atomic utilization and unique catalytic performance of single-atom catalyst (SAC), dual-atomic-site catalysts (DASCs) offer more sophisticated and tunable atomic structure through the modulations of another adjacent metal atom, which can bring new opportunities for CO 2 RR as a deeper extension of SACs and have recently aroused surging interest. In this review, we highlight the recent advances on DASCs for enhancing CO 2 RR. First, the classification, synthesis, and identification of DASCs are provided according to the geometric structure and electronic configuration of dual-atomic active sites. Then, the catalytic applications of DASCs in CO 2 RR are categorized based on marriage-type, hetero-nuclear, and homo-nuclear dual-atomic sites. Particularly, the structure-activity relationship of DASCs in CO 2 RR is elaborately summarized through systematically analyzing the reaction pathways and the atom structures. Finally, the opportunities and challenges are proposed for inspiring the design of future DASCs with high structural accuracy and high CO 2 RR activity and selectivity.

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“…In particular, as a greenhouse gas, excess CO 2 emission results in a severe increase in the global ambient temperature [2][3][4][5]. The renewable energy-driven electrochemical reduction of CO 2 to high-valueadded chemicals, such as CO [6][7][8][9], HCOOH [10,11], CH 4 [12], CH 3 OH [13], and C 2 products [14,15], has been considered an environmentally viable and economic strategy for alleviating the abovementioned issues [16][17][18]. As evaluated from the technoeconomic prospect, formic acid presently has the highest net value, and it is easy to store and transport as a liquid product [19].…”

Section: Introductionmentioning

confidence: 99%

Lattice strain and interfacial engineering of a Bi-based electrocatalyst for highly selective CO2 electroreduction to formate

Wei

Jang

et al. 2022

Sci. China Mater.

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Surface strain tuning in a coupled heterostructure efficiently engineers the catalytic performance of heterogeneous catalysts by altering the electronic structures and boosting electron transport. Generally, Bi-based catalysts are more favorable than ZnO for CO 2 electroreduction to formate, but Bi is much more costly than Zn. Herein, a new Bi 2 O 2 CO 3 /ZnO heterojunction catalyst with porous nanoplate morphology is synthesized through a hexadecyl trimethyl ammonium bromide-templated hydrothermal reaction for a highly efficient catalytic CO 2 reduction reaction (CO 2 RR) to produce formate. The Bi 2 O 2 CO 3 /ZnO catalyst shows a maximum Faradaic efficiency of 92% for formate production at −1.0 V vs. reversible hydrogen electrode (RHE) and a large partial current density of −200 mA mg Bi −1 at −1.2 V vs. RHE. More importantly, the mass activity of Bi 2 O 2 CO 3 /ZnO normalized by Bi mass is an approximately 3.1-fold enhancement over that of the pristine Bi 2 O 2 CO 3 at −1.2 V vs. RHE. By coupling X-ray photoelectron spectroscopy and adsorption spectroscopy measurements, the charge transfer from the Zn atom to the Bi atom through a heterogeneous interface results in an electron-enriched Bi 2 O 2 CO 3 surface, which facilitates CO 2 capture and activation. Meanwhile, compressive stress produced on the catalyst surface helps optimize the adsorption energy of the reaction intermediate, synergistically enhancing the catalytic selectivity and activity of Bi 2 O 2 CO 3 /ZnO for electrochemical CO 2 reduction to formate.

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Bimetallic phthalocyanine heterostructure used for highly selective electrocatalytic CO2 reduction

Cited by 44 publications

References 65 publications

Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction

Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Lattice strain and interfacial engineering of a Bi-based electrocatalyst for highly selective CO2 electroreduction to formate

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Bimetallic phthalocyanine heterostructure used for highly selective electrocatalytic CO2 reduction

Cited by 44 publications

References 65 publications

Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO2 Electroreduction

Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO2 Electroreduction

Emerging dual-atomic-site catalysts for electrocatalytic CO2 reduction

Lattice strain and interfacial engineering of a Bi-based electrocatalyst for highly selective CO2 electroreduction to formate

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Product

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Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction

Modulating the Asymmetric Atomic Interface of Copper Single Atoms for Efficient CO₂ Electroreduction