Effect of mass transfer and kinetics in ordered Cu-mesostructures for electrochemical CO2 reduction

Choi

2019

The Chemical Record

Electrochemical reduction of carbon dioxide (CO2) to valuable organic compounds is promising as to recycling of carbon source of CO2 and technical compatibility with systems using renewable energy resources. In recent years, considerable efforts have been devoted to the research field of CO2 conversion using electrocatalysis. This personal account particularly focuses on the recent progress that has been achieved by the Ertl Center and a number of groups in South Korea that becomes one of the larger CO2 emitters. The research trends of catalyst development divided into different categories according to the primary products are presented first. Afterwards, several studies on theoretical calculations and electrolytic reactors are reviewed taking into account the fundamental understanding and feasibility of the CO2 electroreduction. Finally, a perspective on the challenges and needs in achieving the advanced level of research and development is presented.

Section: P E R S O N a L A C C O U N T T H E C H E M I C A L R E C O R Dmentioning

confidence: 99%

Section: Research Trends In Electrochemical Reduction Of Co2 At the Ementioning

confidence: 99%

Looking Back and Looking Ahead in Electrochemical Reduction of CO₂

Choi

2019

The Chemical Record

“…To tune selectivity, nano-structured Cu electrodes were studied, including Cu nanofoams [155], Cu nanowires [156][157][158][159][160], nanoporous Cu film [161], Cu nanocubes [151][152][153], Cu truncated nanocubes [153], Cu rhombic dodecahedrons [153], inverse opal Cu film [162], mesoporous Cu film [163], electro-redeposited Cu [164], electrodeposited Cu dendrites [165], prism shaped Cu [166], nano-structured Cu by battery cycling [150], hierarchical Cu pillar electrode [167], oxide derived Cu [160,[168][169][170]. The best CO 2 RR performance on Cu electrode was 60~70% faraday efficiency toward C 2 H 4 production [170,171].…”

Section: Metal Producing Multi-carbon Species: Cumentioning

confidence: 99%

Heterogeneous catalysts for catalytic CO2 conversion into value-added chemicals

et al. 2019

As climate change becomes increasingly evident, reducing greenhouse gases including CO 2 has received growing attention. Because CO 2 is thermodynamically very stable, its conversion into value-added chemicals such as CO, CH 4 , or C 2 H 4 is difficult, and developing efficient catalysts for CO 2 conversion is important work. CO 2 can be converted using the gas-phase reaction, liquid-phase reaction, photocatalytic reaction, or electrochemical reaction. The gas-phase reaction includes the dry reforming of methane using CO 2 and CH 4 , or CO 2 hydrogenation using CO 2 and H 2. The liquid-phase reaction includes formic acid formation from pressurized CO 2 and H 2 in aqueous solution. The photocatalytic reaction is commonly known as artificial photo-synthesis, and produces chemicals from CO 2 and H 2 O under light irradiation. The electrochemical reaction can produce chemicals from CO 2 and H 2 O using electricity. In this review, the heterogeneous catalysts used for the gas-phase reaction or electrochemical reactions are discussed, because the liquid-phase reaction and photocatalytic reaction typically suffer from low productivity and poor durability. Because the gas-phase reaction requires a high reaction temperature of > 600°C, obtaining good durability is important. The strategies for designing catalysts with good activity and durability will be introduced. Various materials have been tested for electrochemical conversion, and it has been shown that specific metals can produce specific products, such as Au or Ag for CO, Sn or Bi for formate, Cu for C 2 H 4. Other unconventional catalysts for electrochemical CO 2 reduction are also introduced.

“…Carbon‐based catalysts have been widely used in all kinds of electrochemical reactions for energy conversion on the basis of their tunable surface chemistry, structural diversity, large electron mobility and low cost . Among these reactions, electrochemical CO 2 reduction reaction (CDRR) attracted great research interests recently because it is an approach to consuming CO 2 and producing value‐added fuels or chemicals concurrently . Expectedly, heteroatom‐doped carbons, such as single doping carbons (N−C, F−C) and multiple doping carbons (Si−C−N, NS−C, Fe(Ni, Co)−N−C, Ni(Mn)−Fe−N), and defective carbons were reported as electrocatalysts in this burgeoning field.…”

Section: Introductionmentioning

confidence: 99%

“…[1][2][3][4] Among these reactions, electrochemical CO 2 reduction reaction (CDRR) attracted great research interests recently because it is an approach to consuming CO 2 and producing value-added fuels or chemicals concurrently. [5][6][7] Expectedly, heteroatom-doped carbons, such as single doping carbons (NÀ C, [8][9][10][11] FÀ C [12] ) and multiple doping carbons (SiÀ CÀ N, [13] NSÀ C, [14] Fe(Ni, Co)À NÀ C, [15][16][17][18] Ni (Mn)À FeÀ N [19,20] ), and defective carbons [21][22][23] were reported as electrocatalysts in this burgeoning field. The promoting effects by heteroatom incorporation in carbons were mainly concluded to be the modified orbital energy level via altering charge/spin distribution, as well as the reduced band gap for formation of highly active centers.…”

Section: Introductionmentioning

confidence: 99%

Metal‐Modulated Nitrogen‐Doped Carbon Electrocatalyst for Efficient Carbon Dioxide Reduction

et al. 2020

Carbon‐based catalysts have been increasingly studied for electrochemical CO2 reduction, and their design is mainly focused on modulation of heteroatom dopants, of which chemical states rely highly on the synthesis approach and precursor used. In this work, we present a nitrogen‐doped carbon (NC) catalyst with modulation of N assembled states by Fe particles. The synthetic NC@Fe electrocatalyst enabled efficient and durable CO2 reduction at the maximum CO Faradaic efficiency of 90.6 % and 93 % reservation of its initial activity after long‐term electrolysis. Studies from experiments and DFT calculations indicated that Fe particles induced formation of N‐doped carbon layers in NC@Fe electrocatalyst. These N‐doped carbon layers provide more N‐assembled domains on the surface, in which the triple graphitic N, triple pyridinic N and graphitic‐pyrrolic N configurations were revealed to reduce the formation energy of key intermediates *COOH and *CO for efficient CO2‐to‐CO conversion. These results are hoped to motivate more research on modulation over chemical states of heteroatoms toward synthesis of efficient carbon‐based catalysts for electrocatalytic applications.