Solar energy-driven electrolysis with molecular catalysts for the reduction of carbon dioxide coupled with the oxidation of 5-hydroxymethylfurfural

Yang, Zhi‐Wen; Chen, Jin-Mei; Qiu, Li−Qi; Xie, Wen-Jun; He, Liang‐Nian

doi:10.1039/d2cy01195f

Cited by 16 publications

(11 citation statements)

References 43 publications

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“…used 4‐(tert butyl)‐phenoxy‐decorated cobalt phthalocyanine (TBP‐CoPc) to catalyze the cathodic reduction of CO 2 to CO coupled with the anodic oxidation of HMF to FDCA catalyzed by pyrene bound 2,2,6,6‐tetramethylpiperidine‐1‐oxy (Py‐TEMPO). Owing to the efficiency of the molecular catalyst, when the cell potential is 2.5 V, the partial voltage decreases to 0.87 V on the anode, with the 90.8 % Faradaic efficiency of FDCA [55] . This study shows that the rational design of catalysts and optimization of electrolysis conditions can further improve the possibility of biomass oxidation replacing anodic OER.…”

Section: Cathodic Co2 Electroreduction Coupled With Anodic Organics E...mentioning

confidence: 82%

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Electrocatalytic Reduction of CO₂ Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Zhong

Huang

Ruan

et al. 2023

Chemistry A European J

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The electrochemical process of coupling electrocatalytic CO2 reduction and organic conversion reaction can effectively reduce the reaction overpotential and obtain value‐added chemicals. Moreover, because of the diversity of substrates and the designability of coupling forms, more and more attention has been paid to this field. This review systematically summarizes the research progress of coupling electrolysis in recent years, (1) co‐electrolysis of CO2 and organics at the cathode to obtain specific products with high selectivity, (2) replacing traditional anodic oxygen evolution reaction (OER) with other valuable oxidation reactions to improve energy utilization efficiency and economic benefits of CO2 conversion, (3) in an electrolytic cell without membrane, the cathode and anode jointly transform CO2 and organics to redox products. We hope that the examples and insights on coupling electrolysis introduced in this review can inspire researchers to further explore and innovate in this direction.

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Section: Cathodic Co2 Electroreduction Coupled With Anodic Organics E...mentioning

confidence: 82%

“…2.5 V, the partial voltage decreases to 0.87 V on the anode, with the 90.8 % Faradaic efficiency of FDCA. [55] This study shows that the rational design of catalysts and optimization of electrolysis conditions can further improve the possibility of biomass oxidation replacing anodic OER.…”

Section: Alternative Oxidation Reactionsmentioning

confidence: 89%

Electrocatalytic Reduction of CO₂ Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Zhong

Huang

Ruan

et al. 2023

Chemistry A European J

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“…57,58 Guided by this, we paired ECO 2 RR and 5-hydroxymethylfurfural (HMF) oxidation using the noncovalently immobilized 4-(tert-butyl)-phenoxy cobalt phthalocyanine (TBP-CoPc) and pyrene-tethered 2,2,6,6-tetramethylpiperidin-1-oxy (Py-TEMPO) on carbon nanotubes (CNTs) as electrocatalysts, respectively (Figure 16A). 59,60 These two supported catalysts can be used in the electrolytic cell with trielectrode or dielectrode configuration (Figure 16B and 16C). Even with the cell voltage input from the solar panel, 95.4% selectivity and a turnover number of 52 172 for CO and a 69.9% yield of 2,5furandicarboxylic acid (FDCA) can still be achieved.…”

Section: Electrocatalytic Co 2 Valorization Integrated With Organic S...mentioning

confidence: 99%

Incorporating Catalytic Units into Nanomaterials: Rational Design of Multipurpose Catalysts for CO₂ Valorization

Qiu

2023

Acc. Chem. Res.

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Metrics & MoreArticle Recommendations CONSPECTUS: CO 2 conversion to valuable chemicals is effective at reducing CO 2 emissions. We previously proposed valorization strategies and developed efficient catalysts to address thermodynamic stability and kinetic inertness issues related to CO 2 conversion. Earlier, we developed molecular capture reagents and catalysts to integrate CO 2 capture and conversion, i.e., in situ transformation. Based on the mechanistic understanding of CO 2 capture, activation, and transformation at a molecular level, we set out to develop heterogeneous catalysts by incorporating catalytic units into nanomaterials via the immobilization of active molecular catalysts onto nanomaterials and designing nanomaterials with intrinsic catalytic sites.In thermocatalytic CO 2 conversion, carbonaceous and metal−organic framework (MOF)based catalysts were developed for nonreductive and reductive CO 2 conversion. Novel Cu-and Zn-based MOFs and carbon-supported Cu catalysts were prepared and successfully applied to the cycloaddition, carboxylation, and carboxylative cyclization reactions with CO 2 , generating cyclic carbonates, carboxyl acids, and oxazolidinones as respective target products. Reductive conversion of CO 2 , especially reductive functionalization with CO 2 , is a promising transformation strategy to produce valuable chemicals, alleviating chemical production that relies on petrochemistry. We explored the hierarchical reductive functionalization of CO 2 using organocatalysts and proposed strategies to regulate the CO 2 reduction level, triggering heterogeneous catalyst investigation. Introducing multiple active sites into nanomaterials opens possibilities to develop novel CO 2 transformation strategies. CO 2 capture and in situ conversion were realized with an N-doped carbon-supported Zn complex and MOF materials as CO 2 adsorbents and catalysts. These nanomaterial-based catalysts feature high stability and excellent efficiency and act as shape-selective catalysts in some cases due to their unique pore structure. Nanomaterial-based catalysts are also appealing candidates for photocatalytic CO 2 reduction (PCO 2 RR) and electrocatalytic CO 2 reduction (ECO 2 RR), so we developed a series of hybrid photo-/electrocatalysts by incorporating active metal complexes into different matrixes such as porous organic polymers (POPs), metal−organic layers (MOLs), micelles, and conducting polymers. By introducing Re-bipyridine and Fe-porphyrin complexes into POPs and regulating the structure of the polymer chain, catalyst stability and efficiency increased in PCO 2 RR. PCO 2 RR in aqueous solution was realized by designing the Re-bipyridine-containing amphiphilic polymer to form micelles in aqueous solution and act as nanoreactors. We prepared MOLs with two different metallic centers, i.e., the Ni-bipyridine site and Ni-O node, to improve the efficiency for PCO 2 RR due to the synergistic effect of these metal centers. Sulfylphenoxy-decorated cobalt phthalocyanine (CoPc) cross-linked polypyrrole was prep...

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“…From an energy efficiency point of view, it is important to emphasize coupling the events in both half cells. Although less emphasized in this review, it is preferable to conduct paired redox reactions for the full utilization of the cathode and anode. ,− For example, a value-added process (i.e., CO 2 to syngas) in the counter chamber can be coupled with a targeted reaction to reduce the energy loss during electrolysis (Figure ). A similar strategy was applied using a bifunctional cobalt-modified electrode to achieve simultaneous CO 2 reduction and water splitting .…”

Section: Summary and Outlookmentioning

confidence: 99%

Tuning Electrode Reactivity through Organometallic Complexes

Shen

Wang

et al. 2023

ACS Appl. Mater. Interfaces

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The use of molecularly modified electrodes in catalysis heralds a new paradigm in designing chemical transformations by allowing control of catalytic activity. Herein, we provide an overview of reported methods to develop electrodes functionalized with organometallic complexes and a summary of commonly used techniques for characterizing the electrode surface after immobilization. In addition, we highlight the implications of surface functionalization in catalysis to emphasize the key aspects that should be considered during the development and optimization of functionalized electrodes. Particularly, surface−molecule electronic coupling and electrostatic interactions within a hybrid system are discussed to present effective handles in tuning catalytic activity. We envision that this emerging type of hybrid catalytic system has the potential to combine the advantages of homogeneous catalysis and heterogeneous supports and could be applied to an expanded range of transformations beyond energy conversion.

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Solar energy-driven electrolysis with molecular catalysts for the reduction of carbon dioxide coupled with the oxidation of 5-hydroxymethylfurfural

Abstract: One paired electrolytic system was constructed with 4-(tert-butyl)phenoxy decorated cobalt phthalocyanine (TBP-CoPc) and pyrene-tethered 2,2,6,6-tetramethylpiperidin-1-oxy (Py-TEMPO), which were non-covalently immobilized on carbon nanotubes to catalyze the CO2 reduction to CO...

Cited by 16 publications

References 43 publications

Electrocatalytic Reduction of CO₂ Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Electrocatalytic Reduction of CO₂ Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Incorporating Catalytic Units into Nanomaterials: Rational Design of Multipurpose Catalysts for CO₂ Valorization

Tuning Electrode Reactivity through Organometallic Complexes

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Solar energy-driven electrolysis with molecular catalysts for the reduction of carbon dioxide coupled with the oxidation of 5-hydroxymethylfurfural

Abstract: One paired electrolytic system was constructed with 4-(tert-butyl)phenoxy decorated cobalt phthalocyanine (TBP-CoPc) and pyrene-tethered 2,2,6,6-tetramethylpiperidin-1-oxy (Py-TEMPO), which were non-covalently immobilized on carbon nanotubes to catalyze the CO2 reduction to CO...

Cited by 16 publications

References 43 publications

Electrocatalytic Reduction of CO2 Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Electrocatalytic Reduction of CO2 Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Incorporating Catalytic Units into Nanomaterials: Rational Design of Multipurpose Catalysts for CO2 Valorization

Tuning Electrode Reactivity through Organometallic Complexes

Contact Info

Product

Resources

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Electrocatalytic Reduction of CO₂ Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Electrocatalytic Reduction of CO₂ Coupled with Organic Conversion to Selectively Synthesize High‐Value Chemicals

Incorporating Catalytic Units into Nanomaterials: Rational Design of Multipurpose Catalysts for CO₂ Valorization