Strategies in catalysts and electrolyzer design for electrochemical CO<sub>2</sub>reduction toward C<sub>2+</sub>products

Fan, Lei; Xia, Chuan; Yang, Fubin; Wang, Jun; Wang, Haotian; Lü, Yingying

doi:10.1126/sciadv.aay3111

Cited by 595 publications

(456 citation statements)

References 133 publications

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“…[ 6 ] Nonetheless, the Faradaic efficiency (FE) for CO 2 ‐to‐alcohol production generally remains low, typically less than 50%. [ 7 ] For instance, Gewirth and co‐workers presented a nanoporous Cu–Ag alloy for the enhancement of ECR activity, with an FE toward ethanol of ≈25%. [ 8 ] Bell and co‐workers reported a Cu–Ag alloy with stain effect, and the total FE of alcohol production was less than 15%.…”

Section: Introductionmentioning

confidence: 99%

Electron‐Deficient Cu Sites on Cu₃Ag₁ Catalyst Promoting CO₂ Electroreduction to Alcohols

Shang

Zhou

et al. 2020

Advanced Energy Materials

143

103

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carbon sources through different technical routes, [1] which either have negative environmental impacts or deliver a poor atomic economy while being energy intensive. [2] For instance, the life-cycle greenhouse gas emission for producing a liter of bioethanol is ≈1.6 kg CO 2 equivalent. [3] For fuel ethanol with a global production of ≈104 billion liters per year, [4] the annual CO 2 emission is more than 170 million metric tons, corresponding to 0.5% of the global annual overall carbon emission. [5] New technologies are thus in demand to balance the target of environmental protection and economic development. Electrochemical CO 2 reduction (ECR) driven by renewable energies is a competitive candidate, as it converts CO 2 into liquid products like formate and alcohols with nearly net-zero CO 2 emissions. [6] Nonetheless, the Faradaic efficiency (FE) for CO 2-to-alcohol production generally remains low, typically less than 50%. [7] For instance, Gewirth and co-workers presented a nanoporous Cu-Ag alloy for the enhancement of ECR activity, with an FE toward ethanol of ≈25%. [8] Bell and co-workers reported a Cu-Ag alloy with stain effect, and the total FE of alcohol production was less than 15%. [9] Recently, Sargent and co-workers reported an enhancement of ethanol selectivity in a flow cell system by tuning binding site diversity in an Ag/ Cu catalyst, while the FE for ethanol was still less than 50%. [10] The challenge in developing effective strategies of tuning the energetics of reaction pathways limits the CO 2-to-alcohol selectivity. Based on the theoretical and experimental studies, [11] ethylene (C 2 H 4) generally dominates the C 2+ product distribution, with a theoretical prediction of an alcohol/ethylene ratio of 35:65. [12] However, Calle-Vallejo and Koper reported that ethanol presents a lower free energy position compared to ethylene in the entire reaction route of carbon monoxide (CO) electroreduction to C 2 products. [13] The poor alcohol selectivity has been attributed to the unfavorable adsorption of key intermediates in the ethanol pathway on copper, [13] such as CH 3 CHO* and CH 3 CH 2 O* proved by Chorkendorff and co-workers. [14] Thus, it is rational to hypothesize that an enhanced alcohol selectivity may arise from modulating the adsorption of key intermediates like CH 3 CH 2 O* in the ECR pathways. In addition, it is also well known that Ag component can suppress hydrogen Copper-based catalysts electrochemically convert CO 2 into multicarbon molecules. However, the selectivity toward alcohol products has remained relatively low, due to the lack of catalysts favoring the adsorption of key intermediates in the alcohol pathways. Herein, a Cu 3 Ag 1 electrocatalyst is developed using galvanic replacement of an electrodeposited Cu matrix. The Cu 3 Ag 1 electrocatalyst enables a 63% Faradaic efficiency for CO 2-to-alcohol production and an alcohol partial current density of −25 mA cm −2 at −0.95 V versus reversible hydrogen electrode, corresponding to a 126-fold enhancement in selectivity and 25-...

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Section: Introductionmentioning

confidence: 99%

Electron‐Deficient Cu Sites on Cu₃Ag₁ Catalyst Promoting CO₂ Electroreduction to Alcohols

Shang

Zhou

et al. 2020

Advanced Energy Materials

143

103

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“…Excessive emission of carbon dioxide (CO 2 ) is a threat to the ecological balance. [1][2][3][4][5] CO 2 is also an exploitable carbon and oxygen resource. [6][7][8][9][10][11][12] Fixation of CO 2 into valuable chemicals could simultaneously realize carbon reduction and reutilization of CO 2.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Fixation of Carbon Dioxide in Molten Salts on Liquid Zinc Cathode to Zinc@Graphitic Carbon Spheres for Enhanced Energy Storage

Xiao

Weng

et al. 2020

Advanced Energy Materials

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to epoxides is realized in ionic liquids by Sun and co-workers. [14,15] Fixation and utilization of CO 2 is also elaborately explored via designing the metal-CO 2 batteries by Ding and co-workers. [16] Fixation of CO 2 into functional carbonaceous materials by capture and electrochemical reduction of CO 2 in molten salts has many advantages. [6,17-19] CO 2 shows a high solubility in molten salts, guaranteeing a highflux uptake rate for a direct and deep removal of CO 2 from atmosphere and industrial flue gas. [6] The wide electrochemical window of molten salt electrolytes promises a high current efficiency of the electrochemical reduction of CO 2 in molten salts. [6,20-24] The high-temperature environment of inorganic molten salts brings about enhanced mass transfer and facilitated reaction kinetics, enabling an appealing conversion rate of CO 2 free of any precious catalysts. [6,14,15] Molten salts possess a high heat capacity, which means the heat required by the molten salt fixation of CO 2 can be supplied by solar-thermal systems. [17] The decomposition voltage of CO 2-capture-generated CO 3 2− in molten salts is lower than 2.0 V (1.3 V for Li 2 CO 3 , 1.6 V for Na 2 CO 3 , and 1.8 V for K 2 CO 3 at 500 °C), therefore the electricity for the conversion of CO 2 in molten salts can be supplied by solar photovoltaic systems. [17] Finally, oxygen in CO 2 can simultaneously be released as anodic O 2 , which is of prime implications on future colony on Mars. [6] One of the major challenges for the electrochemical fixation of CO 2 in molten salts is the insufficient functionality of the deposited carbon on cathode. [6] Amorphous and disordered carbon is commonly obtained by electrochemical conversion of CO 2 in molten salts, which contradicts with the demands of application devices for carbonaceous materials with high graphitization degree. [6] For example, aluminum-ion (Al-ion) battery (AIB) possesses the merits of low cost, high volumetric capacity, and high safety. Many cathode materials are reported for Al-ion batteries, including carbon-based materials, metal sulfides, and V 2 O 5. [25-27] For carbon-based materials, the carbon with higher graphitization degree commonly possesses better performance for reversible Al storage. [26,27] In this regard, pioneering works were conducted by Lu and coworkers. [7,28-33] In their strategy, a highly porous 3D graphene foam is used as the cathode for rechargeable Al-ion batteries,

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“…With the developed of design for ECR catalysts, recent studies have begun to reduce CO 2 into CH 4 , CH 3 OH, HCHO, and high-density C 2+ products, and some research progress has been made in the reaction mechanism of ECR into these products. For the mechanism of ECR to CH 4 , CH 3 OH, and HCHO, theoretical and experimental studies [46]. Based on the in-depth understanding of the mechanism of ECR, low-cost electrocatalysts with excellent catalytic activity, high selectivity, and long durability are required to realize the large-scale application of ECR technology.…”

Section: Mechanism Of Ecrmentioning

confidence: 99%

Defect Engineering on Carbon-Based Catalysts for Electrocatalytic CO2 Reduction

et al. 2020

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Electrocatalytic carbon dioxide (CO2) reduction (ECR) has become one of the main methods to close the broken carbon cycle and temporarily store renewable energy, but there are still some problems such as poor stability, low activity, and selectivity. While the most promising strategy to improve ECR activity is to develop electrocatalysts with low cost, high activity, and long-term stability. Recently, defective carbon-based nanomaterials have attracted extensive attention due to the unbalanced electron distribution and electronic structural distortion caused by the defects on the carbon materials. Here, the present review mainly summarizes the latest research progress of the construction of the diverse types of defects (intrinsic carbon defects, heteroatom doping defects, metal atomic sites, and edges detects) for carbon materials in ECR, and unveil the structure–activity relationship and its catalytic mechanism. The current challenges and opportunities faced by high-performance carbon materials in ECR are discussed, as well as possible future solutions. It can be believed that this review can provide some inspiration for the future of development of high-performance ECR catalysts.

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Strategies in catalysts and electrolyzer design for electrochemical CO₂reduction toward C₂₊products

Cited by 595 publications

References 133 publications

Electron‐Deficient Cu Sites on Cu₃Ag₁ Catalyst Promoting CO₂ Electroreduction to Alcohols

Electron‐Deficient Cu Sites on Cu₃Ag₁ Catalyst Promoting CO₂ Electroreduction to Alcohols

Electrochemical Fixation of Carbon Dioxide in Molten Salts on Liquid Zinc Cathode to Zinc@Graphitic Carbon Spheres for Enhanced Energy Storage

Defect Engineering on Carbon-Based Catalysts for Electrocatalytic CO2 Reduction

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Strategies in catalysts and electrolyzer design for electrochemical CO2reduction toward C2+products

Cited by 595 publications

References 133 publications

Electron‐Deficient Cu Sites on Cu3Ag1 Catalyst Promoting CO2 Electroreduction to Alcohols

Electron‐Deficient Cu Sites on Cu3Ag1 Catalyst Promoting CO2 Electroreduction to Alcohols

Electrochemical Fixation of Carbon Dioxide in Molten Salts on Liquid Zinc Cathode to Zinc@Graphitic Carbon Spheres for Enhanced Energy Storage

Defect Engineering on Carbon-Based Catalysts for Electrocatalytic CO2 Reduction

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Strategies in catalysts and electrolyzer design for electrochemical CO₂reduction toward C₂₊products

Electron‐Deficient Cu Sites on Cu₃Ag₁ Catalyst Promoting CO₂ Electroreduction to Alcohols

Electron‐Deficient Cu Sites on Cu₃Ag₁ Catalyst Promoting CO₂ Electroreduction to Alcohols