Well-Defined Nanographene–Rhenium Complex as an Efficient Electrocatalyst and Photocatalyst for Selective CO<sub>2</sub> Reduction

Qiao, Xiaoxiao; Li, Qiqi; Schaugaard, Richard N.; Noffke, Benjamin W.; Liu, Yijun; Li, Dongping; Liu, Lu; Raghavachari, Krishnan; Li, Liang-shi

doi:10.1021/jacs.6b12530

Cited by 101 publications

(94 citation statements)

References 40 publications

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“…2019, 9,1900090 Figure 32. [90][91][92][93][94][95][96] While electroreduction of CO 2 involving copper has mainly focused on multielectron transfers at copper electrodes to produce products such as methanol (6 electron reduced) as compared to CO and HCOOH (2 electron reduced), Cu molecular catalysts have also been researched in a heterogeneous form to produce similar products. HER at pH = 1 (black curve), pH = 2 (red curve) and pH = 3 (blue curve) on Co protoporphyrin-modified PG electrode in the absence of CO 2 .…”

Section: Other Metal-based Catalystsmentioning

confidence: 99%

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Elouarzaki

Kannan

Jose

et al. 2019

Advanced Energy Materials

168

102

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provides a promising alternative to hydrocarbon sources for petrochemical feedstock. Thanks to the electrochemical nature of the CO 2 conversion to fuels and chemicals, the electrical energy invested to convert CO 2 in the form of a chemical fuel can be stored and redistributed using established supply chains for future use. Additionally, the integration of renewable energy systems (green electricity) into the grid can potentially create a carbon neutral energy cycle, and when driven by solar energy, offers a completely renewable energy cycle or negative carbon technology. Converting CO 2 electrochemically into compounds with high energy densities, such as alcohols (methanol, ethanol), formates, and CO, represents a form of energy storage and is also adaptable to demand response or energy arbitrage technologies. [3][4][5][6][7] The recoverable energy density of the chemicals that can be converted from CO 2 is substantially higher than most battery technologies.Given CO 2 electroreduction's immense economic and environmental potential, it has been the subject of much research activity over the past decades. [8][9][10][11] One of the greatest challenges of reducing CO 2 in an electrochemical cell is overcoming the immense energy barrier required to do so; the single electron reduction of CO 2 to CO 2 −˙, a common step in many CO 2 reduction mechanisms, requires an applied potential of −1.97 V measured versus standard hydrogen electrode (SHE). To alleviate this problem, many catalytic cathodes have been developed to avoid this intermediate and to reroute the reduction mechanism through alternate pathways requiring much lower applied potentials (a necessity if CO 2 electroreduction is to be implemented at industrial scale). [12][13][14] However, despite the low potentials offered by catalytic electrodes, the cost of electrodes is not always viable when upscaled to industrial levels. [15,16] Therefore, recent research trends in electrocatalytic reduction of CO 2 have been shifting toward the development of molecular catalysts that can exist as either solutes in electrolytes or can be surface-confined on electrodes. [13,16] The tunable nature and electronic characteristics of molecular catalysts give access to a large variety of catalysts with high activity, selectivity, and durability, as well as their ability to be integrated into sophisticated nanoassemblies. [17][18][19] Thanks to the aforementioned proprieties, performing CO 2 reduction using molecularly defined compounds offer several advantages compared to classical solid-state counterparts. Molecular catalysts usually exhibit well-defined homogeneous and/or CO 2 reduction using molecular catalysts is a key area of study for achieving electrical-to-chemical energy storage and feedstock chemical synthesis. Compared to classical metallic solid-state catalysts, these molecular catalysts often result in high performance and selectivity, even under unfavorable aqueous environments. This review considers the recent state-of-the-art molecular catalysts for CO 2 electro...

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Section: Other Metal-based Catalystsmentioning

confidence: 99%

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Elouarzaki

Kannan

Jose

et al. 2019

Advanced Energy Materials

168

102

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“…Currently, the proposed methods for reducing the CO 2 content in the atmosphere are mainly focused on two central topics: CO 2 sequestration as and CO 2 conversion and utilization. The former option demands additional energy consumption while causing concerns regarding the ecological safety; the latter option is an ideal method that leverages chemical, photo‐, or electrocatalysis to reduce the CO 2 in atmosphere for incorporation into a usable form of organic matter . In particular, photocatalytic reduction does not require any external electrical or thermal energy.…”

Section: Introductionmentioning

confidence: 99%

Preparation of Cuprous Oxide Nanoparticles Coated with Aminated Cellulose for the Photocatalytic Reduction of Carbon Dioxide to Methanol

et al. 2018

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The present study utilizes microcrystalline cellulose as the raw material to prepare nanoscale cellulose crystal (NCC) particles through a hybrid method incorporating mixed acid and ultrasonic treatment. Furthermore, the NCC undergoes a surface modification through SOCl2 chlorination and ethylenediamine (EDA) passivation, which generates graphitized aminated cellulose doped with nitrogen (NCC‐EDA). This product, due to the coordination and dispersion effects of the functional groups (e.g., amido group) on its surface, is in turn used to coat Cu2O nanoparticles derived from the in situ reduction of CuCl2⋅2 H2O, which leads to a composite photocatalyst Cu2O/NCC‐EDA with relatively high catalytic activity. Besides the structural characterization, the present study also examines the characteristics of CH3OH prepared by visible‐light‐based photocatalytic reduction of CO2/H2O. The results indicate that the prepared Cu2O/NCC‐EDA are spherical particles with a diameter of approximately 50 nm, which are in possession of a tree‐structured rough shell capable of absorbing an increased amount of CO2. Under the radiation of visible light, the Cu2O in the prepared product is activated, yielding photoelectron–hole pairs. Driven by the nitrogen in the carrier, the formed photoelectron–hole pairs are subject to an efficient separation, and are thereby consumed by the oxidation–reduction reaction. As a result, a high activity for the photocatalyzed reduction of CO2 is obtained.

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“…Dies wird bei der Deutung der Ergebnisse des Austauschs,d ie in Gegenwart von Graphen und Carbidnanoschichten gemessen wurden, hilfreich sein. Die Nanomaterialien lassen sich in zwei Gruppen einordnen:i )metallhaltige Photokatalysatoren wie Oxide, [11,39,48,53,54,70,[73][74][75][76][77][78][79][80][81] Chalkogenide, [49] Bismut-Oxyhalogenide, [82][83][84][85][86][87] Hydrotalcite [88] und Zeolithe; [89] ii)metallfreie Photokatalysatoren wie Graphen und seine Derivate (Graphenoxide (GO) und mit Heteroatomen dotiertes Graphen), [55,[90][91][92][93][94][95][96] g-C 3 N 4 [97][98][99][100][101][102] und kohlenstoffdotiertes h-BN. [55,56,72] Die Photoreduktionen von 13 CO 2 zu 13 CH 4 [55] und 13 CH 3 OH [54] wurden ebenfalls beschrieben.…”

Section: Mçgliche Reaktionspfade Der Co 2 -Reduktionunclassified

Katalyse der Kohlenstoffdioxid‐Photoreduktion an Nanoschichten: Grundlagen und Herausforderungen

et al. 2018

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Die Umwandlung von CO2 in Treibstoffe und Chemikalien mithilfe der Photokatalyse ist eine vielversprechende Methode, um die Probleme der globalen Erwärmung und Energieversorgung nachhaltig zu lösen. Erfolge im Bereich der Photokatalyse während des letzten Jahrzehnts haben verstärktes Interesse an der Nutzung des Sonnenlichts zur Reduktion von CO2 hervorgerufen. Traditionelle Halbleiter in der Photokatalyse (z. B. TiO2) sind für die Anwendung in natürlichem Sonnenlicht nicht geeignet und sogar unter UV‐Bestrahlung nicht effizient genug. Kürzlich wurden einige zweidimensionale (2D) Materialien für die katalytische CO2‐Reduktion entwickelt. Diese Materialien müssen noch erheblich verbessert werden, was eine Herausforderung für die Entwicklung photokatalytischer Prozesse darstellt. Hier wird die Literatur über die photokatalytische CO2‐Umwandlung mit 2D‐Materialien in der Flüssigphase zusammengefasst, um eine Grundlage für die Suche nach verbesserten Materialien zu schaffen.

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Well-Defined Nanographene–Rhenium Complex as an Efficient Electrocatalyst and Photocatalyst for Selective CO₂ Reduction

Cited by 101 publications

References 40 publications

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Preparation of Cuprous Oxide Nanoparticles Coated with Aminated Cellulose for the Photocatalytic Reduction of Carbon Dioxide to Methanol

Katalyse der Kohlenstoffdioxid‐Photoreduktion an Nanoschichten: Grundlagen und Herausforderungen

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Well-Defined Nanographene–Rhenium Complex as an Efficient Electrocatalyst and Photocatalyst for Selective CO2 Reduction

Cited by 101 publications

References 40 publications

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO2 by Molecular Catalysts

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO2 by Molecular Catalysts

Preparation of Cuprous Oxide Nanoparticles Coated with Aminated Cellulose for the Photocatalytic Reduction of Carbon Dioxide to Methanol

Katalyse der Kohlenstoffdioxid‐Photoreduktion an Nanoschichten: Grundlagen und Herausforderungen

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Product

Resources

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Well-Defined Nanographene–Rhenium Complex as an Efficient Electrocatalyst and Photocatalyst for Selective CO₂ Reduction

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts