Efficient electrosynthesis of n-propanol from carbon monoxide using a Ag–Ru–Cu catalyst

Wang, Xue; Ou, Pengfei; Ozden, Adnan; Hung, Sung‐Fu; Tam, Jason; Gabardo, Christine M.; Howe, Jane Y.; Sisler, Jared; Bertens, Koen; Arquer, F. Pelayo Garcı́a de; Miao, Rui Kai; O’Brien, Colin P.; Wang, Ziyun; Abed, Jehad; Rasouli, Armin Sedighian; Sun, Meng‐Jia; Ip, Alexander H.; Sinton, David; Sargent, Edward H.

doi:10.1038/s41560-021-00967-7

Cited by 177 publications

(139 citation statements)

References 48 publications

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“…The electrocatalytic reduction of carbon dioxide driven by renewable electricity can convert atmospheric carbon dioxide into value-added fuels and bulk petrochemicals, including carbon monoxide, 16 formic acid, 17 ethylene, 18 ethanol, 19 acetic acid, 20 and n -propanol 21 ( Figure 2 a). The market size for ethylene alone represented 83 billion USD in 2021 and this single chemical accounts for 260 million tons of CO 2 emission per year.…”

Section: Electroreduction Of Co 2 and Co To Petroc...mentioning

confidence: 99%

Emerging Electrochemical Processes to Decarbonize the Chemical Industry

Rong

Overa

Jiao

2022

JACS Au

103

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Electrification is a potential approach to decarbonizing the chemical industry. Electrochemical processes, when they are powered by renewable electricity, have lower carbon footprints in comparison to conventional thermochemical routes. In this Perspective, we discuss the potential electrochemical routes for chemical production and provide our views on how electrochemical processes can be matured in academic research laboratories for future industrial applications. We first analyze the CO 2 emission in the manufacturing industry and conduct a survey of state of the art electrosynthesis methods in the three most emission-intensive areas: petrochemical production, nitrogen compound production, and metal smelting. Then, we identify the technical bottlenecks in electrifying chemical productions from both chemistry and engineering perspectives and propose potential strategies to tackle these issues. Finally, we provide our views on how electrochemical manufacturing can reduce carbon emissions in the chemical industry with the hope to inspire more research efforts in electrifying chemical manufacturing.

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Section: Electroreduction Of Co 2 and Co To Petroc...mentioning

confidence: 99%

Emerging Electrochemical Processes to Decarbonize the Chemical Industry

Rong

Overa

Jiao

2022

JACS Au

103

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“…The dimerization of *CO [46,47] and coupling of *CO with protonated *CO (*CHO or *COH) [48,49] are widely accepted possible routes for C-C coupling. In the *CO dimerization mechanism, C-C coupling is generally regarded as the rate-determining step (RDS) for C 2+ production and has been widely applied in theoretical calculations [50,51]. In this case, two *CO intermediates on the Cu surface are coupled to form *OCCO, and this process is accompanied by an electron transfer [52].…”

Section: Proposed Mechanisms For Co 2 Rr Toward C 2+ Productsmentioning

confidence: 99%

Rational Manipulation of Intermediates on Copper for CO2 Electroreduction Toward Multicarbon Products

Han

Gao

et al. 2022

Trans. Tianjin Univ.

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Excess greenhouse gas emissions, primarily carbon dioxide (CO2), have caused major environmental concerns worldwide. The electroreduction of CO2 into valuable chemicals using renewable energy is an ecofriendly approach to achieve carbon neutrality. In this regard, copper (Cu) has attracted considerable attention as the only known metallic catalyst available for converting CO2 to high-value multicarbon (C2+) products. The production of C2+ involves complicated C–C coupling steps and thus imposes high demands on intermediate regulation. In this review, we discuss multiple strategies for modulating intermediates to facilitate C2+ formation on Cu-based catalysts. Furthermore, several sophisticated in situ characterization techniques are outlined for elucidating the mechanism of C–C coupling. Lastly, the challenges and future directions of CO2 electroreduction to C2+ are envisioned.

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“…[20,21] Early work on CORR obtained a FE in excess of 20% for n-propanol at gas diffusion electrode in a flow cell. [21][22][23][24] Furthermore, an Ag-Ru-Cu alloy catalyst endowed FE of 36% for propanol at the current density of 300 mA cm -2 . [23] Unfortunately, owing to the risk of high-pressure storage of CO and high equipment maintenance cost, it is not realistic to achieve either industrial or decentralized multi-carbon products using CO as a feedstock.Distinct from CO, CO 2 is a safe, cheap, and easily liquefied gas.…”

mentioning

confidence: 99%

“…[21][22][23][24] Furthermore, an Ag-Ru-Cu alloy catalyst endowed FE of 36% for propanol at the current density of 300 mA cm -2 . [23] Unfortunately, owing to the risk of high-pressure storage of CO and high equipment maintenance cost, it is not realistic to achieve either industrial or decentralized multi-carbon products using CO as a feedstock.Distinct from CO, CO 2 is a safe, cheap, and easily liquefied gas. Hence, we propose that a tandem catalytic CO 2 RR system consisting of two independent sections of CO 2 to CO and CO to n-propanol may easily solve the problem of highpressure CO storage.…”

mentioning

confidence: 99%

“…Hence, we propose that a tandem catalytic CO 2 RR system consisting of two independent sections of CO 2 to CO and CO to n-propanol may easily solve the problem of highpressure CO storage. [25] Since the input chemicals account for the largest proportion of cost in CORR industrialization, [23] Electrocatalytic reduction of CO 2 (CO 2 RR) to high-energy-density C 3 fuels like n-propanol has been widely recognized as one of the core technologies for both renewable energy storage and carbon neutrality. Unfortunately, exceptional catalytic sites that are able to simultaneously implement efficient conversion to C 1 and C 2 products are difficult to design for single electrolyzers, leading to poor activity and selectivity toward n-propanol.…”

mentioning

confidence: 99%

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Selective Electroreduction of CO₂ to n‐Propanol in Two‐Step Tandem Catalytic System

Song

Zheng

et al. 2022

Advanced Energy Materials

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Electrocatalytic conversion of CO 2 to chemical fuels serves a two-fold purpose of energy storage and carbon offset. Among those, the efficiency of electrocatalytic reduction of CO 2 to one-carbon (C 1 ) products including CO [1][2][3] and formate [4][5][6] is approaching commercialization, while the transformation of CO 2 to C 2 products such as ethylene [7][8][9][10] and ethanol [11,12] is developing rapidly. In comparison, research on the conversion of CO 2 to high-energy C 3 fuels like n-propanol [13][14][15][16][17][18][19] is seriously lagging behind despite the unique merits of products, e.g., high added value and easy management.Metallic Cu is known to be the only efficient catalyst by far for the electroreduction of CO 2 to n-propanol. Since the pioneering report on electroreduction of CO 2 to n-propanol at Cu electrode in 1988, [14] several strategies of modifying copper-based catalysts, including structural reconstruction, [15] two-step activation, [16] metal ion cycling, [17] core-shell structure [18] and double sulfur vacancies, [19] have been developed, pushing the FE of n-propanol to 15.4% and the partial current density to 10.2 mA cm -2 . Nevertheless, complex design on Cu catalysts are needed, because n-propanol formation involves multiple active sites that are responsible for the reduction of CO 2 to CO intermediate and subsequent carbon-carbon coupling, respectively. Such drawback largely limits the selection of Cu-based catalysts, thus impeding commercial production of n-propanol from CO 2 electroreduction.We notice that direct electrocatalytic reduction of CO (CORR) could considerably promote n-propanol generation. [20,21] Early work on CORR obtained a FE in excess of 20% for n-propanol at gas diffusion electrode in a flow cell. [21][22][23][24] Furthermore, an Ag-Ru-Cu alloy catalyst endowed FE of 36% for propanol at the current density of 300 mA cm -2 . [23] Unfortunately, owing to the risk of high-pressure storage of CO and high equipment maintenance cost, it is not realistic to achieve either industrial or decentralized multi-carbon products using CO as a feedstock.Distinct from CO, CO 2 is a safe, cheap, and easily liquefied gas. Hence, we propose that a tandem catalytic CO 2 RR system consisting of two independent sections of CO 2 to CO and CO to n-propanol may easily solve the problem of highpressure CO storage. [25] Since the input chemicals account for the largest proportion of cost in CORR industrialization, [23] Electrocatalytic reduction of CO 2 (CO 2 RR) to high-energy-density C 3 fuels like n-propanol has been widely recognized as one of the core technologies for both renewable energy storage and carbon neutrality. Unfortunately, exceptional catalytic sites that are able to simultaneously implement efficient conversion to C 1 and C 2 products are difficult to design for single electrolyzers, leading to poor activity and selectivity toward n-propanol. Alternatively, electroreduction of CO (CORR) has shown good performance toward C 3 fuels, but the cost and safety of gas storage h...

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Efficient electrosynthesis of n-propanol from carbon monoxide using a Ag–Ru–Cu catalyst

Cited by 177 publications

References 48 publications

Emerging Electrochemical Processes to Decarbonize the Chemical Industry

Emerging Electrochemical Processes to Decarbonize the Chemical Industry

Rational Manipulation of Intermediates on Copper for CO2 Electroreduction Toward Multicarbon Products

Selective Electroreduction of CO₂ to n‐Propanol in Two‐Step Tandem Catalytic System

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Efficient electrosynthesis of n-propanol from carbon monoxide using a Ag–Ru–Cu catalyst

Cited by 177 publications

References 48 publications

Emerging Electrochemical Processes to Decarbonize the Chemical Industry

Emerging Electrochemical Processes to Decarbonize the Chemical Industry

Rational Manipulation of Intermediates on Copper for CO2 Electroreduction Toward Multicarbon Products

Selective Electroreduction of CO2 to n‐Propanol in Two‐Step Tandem Catalytic System

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Product

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Selective Electroreduction of CO₂ to n‐Propanol in Two‐Step Tandem Catalytic System