Synergistic Catalysis over Iron‐Nitrogen Sites Anchored with Cobalt Phthalocyanine for Efficient CO<sub>2</sub> Electroreduction

Lin, Lanying; Li, Haobo; Yan, Cairong; Li, Hefei; Si, Rui; Li, Mingrun; Xiao, Jianping; Wang, Guoxiong; Bao, Xinhe

doi:10.1002/adma.201903470

Cited by 288 publications

(186 citation statements)

References 33 publications

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“…Electroreduction of CO 2 into fuels and chemical feedstocks is a promising way to alleviate energy crises and greenhouse effect. [1][2][3][4][5] During the process of CO 2 electroreduction, different catalytic products, including carbon monoxide (CO) [6,7] , methane (CH 4 ) [8] , formate (HCOO À ) [9,10] , methanol (CH 3 OH) [11] , ethylene (C 2 H 4 ) [12] , and ethanol (C 2 H 5 OH) [13] , have been obtained. Among these products, CO can be used as cleaner gaseous fuel, as well as raw material for the production of methanol, Fischer-Tropsch synthesis and various organic synthesis.…”

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confidence: 99%

Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO₂ Electroreduction into CO

et al. 2020

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Electroreduction of CO2 into carbonaceous fuels or industrial chemicals using renewable energy sources is an ideal way to promote global carbon recycling. Thus, it is of great importance to develop highly selective, efficient, and stable catalysts. Herein, we prepared cobalt single atoms (Co SAs) coordinated with phthalocyanine (Co SAs‐Pc). The anchoring of phthalocyanine with Co sites enabled electron transfer from Co sites to CO2 effectively via the π‐conjugated system, resulting in high catalytic performance of CO2 electroreduction into CO. During the process of CO2 electroreduction, the Faradaic efficiency (FE) of Co SAs‐Pc for CO was as high as 94.8 %. Meanwhile, the partial current density of Co SAs‐Pc for CO was −11.3 mA cm−2 at −0.8 V versus the reversible hydrogen electrode (vs RHE), 18.83 and 2.86 times greater than those of Co SAs (−0.60 mA cm−2) and commercial Co phthalocyanine (−3.95 mA cm−2), respectively. In an H‐cell system operating at −0.8 V vs RHE over 10 h, the current density and FE for CO of Co SAs‐Pc dropped by 3.2 % and 2.5 %. A mechanistic study revealed that the promoted catalytic performance of Co SAs‐Pc could be attributed to the accelerated reaction kinetics and facilitated CO2 activation.

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Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO₂ Electroreduction into CO

et al. 2020

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“…The dual metal sites consisting of homo-metal species have also demonstrated their superiority in ORR, [75] NRR [76] and alkene epoxidation. [77] Additionally, there is great interest in synthesizing the adjacent dual-metal-site catalysts with different metal species, which has been demonstrated to be highly effective for improved catalytic performance, including Co-Pt, [72] Fe-Pt, [78] Co-Fe, [79] Pt-Ru, [80] and Ni-Fe [81] materials. Yao and co-workers prepared an atomic Co-Pt coupling species on the defective C/N graphene (A-CoPt-NC) through the pyrolysis of Co-based metalorganic frameworks (MOFs) and subsequent electrochemical activation, as evidenced by the HADDF-STEM observations (Figure 4g).…”

Section: Synergy Of Neighboring Single Metal Atomsmentioning

confidence: 99%

Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis

Liu

Ding

et al. 2020

Advanced Energy Materials

210

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Single atom catalysts (SACs) that integrate the merits of homogeneous and heterogeneous catalysts have been attracting considerable attention in recent years. The individual metal atoms of SACs can be stabilized on supports through various unsaturated chemical sites or space confinement for achieving the maximized atom utilization efficiency. Aside from the development of strategies for preparing high loading and high purity SACs, another key challenge in this field is precisely manipulating the geometric and electronic structure of catalytically active single metal sites, thus rendering the catalysts exceptionally reactive, selective, and stabile compared to their bulk counterparts. This review summarizes recent advancements in SACs for heterogeneous catalysis from the perspective of local structural regulation and the synergistic coupling effect between metal species and supports. Special emphasis is placed on the elucidation of the catalytic structure‐performance relationship in terms of coordination environment, valence state and metal‐support interactions by advanced characterization and theoretical studies. Select in situ or operando characterization techniques for tracking the SACs’ structure evolution under realistic conditions are highlighted. Finally, the challenges and opportunities are discussed to offer insight into the rational design of more intriguing SACs with high activity and distinct chemoselectivity.

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“…Besides directly constructing metal‐metal bond, Lin et al improved the reactivity of Fe SACs through constructing a strong interaction between Fe‐ and Co‐based centers in cobalt phthalocyanine anchored Fe–‐N–C substrate. [ 95 ] The composite showed high CO FE above 90% over a wider potential window of 0.71 V than 0.18 V of Fe–N–C alone. Meanwhile, the maximum current density of CO production was increased with enhanced durability.…”

Section: Modifying the Nanostructured Electrocatalysts At Atomic Scalmentioning

confidence: 99%

Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO₂ Reduction

Liu

Zhu

et al. 2020

Adv Funct Materials

110

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Electrochemical reduction of CO 2 into value-added chemicals provides a promising approach to mitigate climate change caused by CO 2 from excess consumption of fossil fuels. As the CO 2 molecule is chemically inert and the reaction kinetics is sluggish, efficient electrocatalysts are thus highly required for promoting the conversion of CO 2 . With great efforts devoted to improving the catalytic performance, the development of electrocatalysts for CO 2 reduction has gone from bulk metals with poor control to nanostructures with atomic precision. Nanostructured electrocatalysts with atomic precision are believed to be capable of combining the advantages of heterogeneous and homogenous catalysts. In this review, the recent advances in designing nanostructured electrocatalysts at the atomic level for boosting the catalytic performance toward CO 2 reduction and revealing the structure-property relationship are summarized. The challenges and opportunities in the near future are also proposed for paving the development of electrocatalytic CO 2 reduction.half reactions and equilibrium potentials (versus reversible hydrogen electrode (RHE)) are listed as Reaction (1) to (6): [7] CO 2H 2e HCOOH 0.12 V Adv. Funct.

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Synergistic Catalysis over Iron‐Nitrogen Sites Anchored with Cobalt Phthalocyanine for Efficient CO₂ Electroreduction

Cited by 288 publications

References 33 publications

Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO₂ Electroreduction into CO

Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO₂ Electroreduction into CO

Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis

Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO₂ Reduction

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Synergistic Catalysis over Iron‐Nitrogen Sites Anchored with Cobalt Phthalocyanine for Efficient CO2 Electroreduction

Cited by 288 publications

References 33 publications

Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO2 Electroreduction into CO

Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO2 Electroreduction into CO

Structural Regulation and Support Coupling Effect of Single‐Atom Catalysts for Heterogeneous Catalysis

Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO2 Reduction

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Synergistic Catalysis over Iron‐Nitrogen Sites Anchored with Cobalt Phthalocyanine for Efficient CO₂ Electroreduction

Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO₂ Electroreduction into CO

Molecular Modification of Single Cobalt Sites Boosts the Catalytic Activity of CO₂ Electroreduction into CO

Recent Advances in Atomic‐Level Engineering of Nanostructured Catalysts for Electrochemical CO₂ Reduction