Copper-Tin Alloys for the Electrocatalytic Reduction of CO2 in an Imidazolium-Based Non-Aqueous Electrolyte

The ability to synthesize value-added chemicals directly from CO2 will be an important technological advancement for future generations. Using solar energy to drive thermodynamically uphill electrochemical reactions allows for near carbon-neutral processes that can convert CO2 into energy-rich carbon-based fuels. Here, we report on the use of inexpensive CuSn alloys to convert CO2 into CO in an acetonitrile/imidazolium-based electrolyte. Synergistic interactions between the CuSn catalyst and the imidazolium cation enables the electrocatalytic conversion of CO2 into CO at −1.65 V versus the standard calomel electrode (SCE). This catalyst system is characterized by overpotentials for CO2 reduction that are similar to more expensive Au- and Ag-based catalysts, and also shows that the efficacy of the CO2 reduction reaction can be tuned by varying the CuSn ratio.

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Non-metal photochemical reduction of CO2 to formate with organohydride-recycle strategy

10.26434/chemrxiv-2021-ch3ts ◽

2021 ◽

Author(s):

Weibin Xie ◽

Jiasheng Xu ◽

Ubaidah Md Idros ◽

Jouji Katsuhira ◽

Masaaki Fuki ◽

...

Keyword(s):

Co2 Reduction ◽

Co2 Concentration ◽

Catalyst System ◽

High Energy ◽

Global Scale ◽

Reduction Reaction ◽

Photochemical Reduction ◽

Catalyst Systems ◽

Reduction Of Co2 ◽

Co2 Reduction Reaction

The increasing CO2 concentration in the atmosphere is an urgent social problem that has to be resolved. Reducing CO2 into compounds useful as energy sources and carbon materials is desirable. For the CO2 reduction reaction (CO2RR) to be operational on a global scale, the catalyst system must: (1) use only renewable energy, (2) be built from abundantly available elements, and (3) not require high-energy reactants. Although light is an alluring energy source, most existing methods utilize electricity. Furthermore, catalyst systems are based on rare heavy metals. Herein, we present a transition-metal-free catalyst system for CO2RR using visible light and containing a carbazole photocatalyst and an organohydride co-catalyst based on benzimidazoline. It produced formate with a turnover number exceeding 8000. No other reduced products such as H2 and CO were generated, confirming the high selectivity of the system. This finding is essential for operating artificial photosynthesis on a useful scale.

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Investigation of Zn/Ni-Based Electrocatalysts for Electrochemical Conversion of CO2 to SYNGAS

10.5772/intechopen.95626 ◽

2021 ◽

Author(s):

Mohammadali Beheshti ◽

Saeid Kakooei ◽

Mokhtar Che Ismail ◽

Shohreh Shahrestani

Keyword(s):

Large Scale ◽

Steel Substrate ◽

Renewable Energy Sources ◽

Coke Formation ◽

Co2 Reduction ◽

Value Added ◽

Reduction Reaction ◽

Electrochemical Tests ◽

Reduction Of Co2 ◽

Co2 Reduction Reaction

In the last decade, there is some research on the conversion of CO2 to energy form. CO2 can be converted to value-added chemicals including HCOOH, CO, CH4, C2H4, and liquid hydrocarbons that can be used in various industries. Among the methods, electrochemical methods are of concern regarding their capability to operate with an acceptable reaction rate and great efficiency at room temperature and can be easily coupled with renewable energy sources. Besides, electrochemical cell devices have been manufactured in a variety of sizes, from portable to large-scale applications. Catalysts that optionally reduce CO2 at low potential are required. Therefore, choosing a suitable electrocatalyst is very important. This chapter focused on the electrochemical reduction of CO2 by Zn-Ni bimetallic electrocatalyst. The Zn-Ni coatings were deposited on the low-carbon steel substrate. Electrochemical deposition parameters such as temperature in terms of LPR corrosion rate, microstructure, microcracks, and its composition have been investigated. Then, the electrocatalyst stability and activity, as well as gas intensity and selectivity, were inspected by SEM/EDX analysis, GC, and electrochemical tests. Among the electrocatalysts for CO2 reduction reaction, the Zn65%-Ni35% electrode with cluster-like microstructure had the best performance for CO2 reduction reaction according to minimum coke formation (<10%) and optimum CO and H2 faradaic efficiencies (CO FE% = 55% and H2 FE% = 45%).

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Graphene Supported Tungsten Carbide as Catalyst for Electrochemical Reduction of CO2

10.26434/chemrxiv.8280986 ◽

2019 ◽

Author(s):

Sahithi Ananthaneni ◽

Rees Rankin

Keyword(s):

Tungsten Carbide ◽

Electrochemical Reduction ◽

Low Cost ◽

Co2 Reduction ◽

Platinum Group Metal ◽

Reduction Reaction ◽

Metal Carbides ◽

Depth Study ◽

Reduction Of Co2 ◽

Co2 Reduction Reaction

<div>Electrochemical reduction of CO2 to useful chemical and fuels in an energy efficient way is currently an expensive and inefficient process. Recently, low-cost transition metal-carbides (TMCs) are proven to exhibit similar electronic structure similarities to Platinum-Group-Metal (PGM) catalysts and hence can be good substitutes for some important reduction reactions. In this work, we test graphenesupported WC (Tungsten Carbide) nanocluster as an electrocatalyst for the CO2 reduction reaction. Specifically, we perform DFT studies to understand various possible reaction mechanisms and determine the lowest thermodynamic energy landscape of CO2 reduction to various products such as CO, HCOOH, CH3OH, and CH4. This in-depth study of reaction energetics could lead to improvements and develop more efficient electrocatalysts for CO2 reduction.<br></div>

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Three-dimensional porous copper-decorated bismuth-based nanofoam for boosting electrochemical reduction of CO2 to formate

Inorganic Chemistry Frontiers ◽

10.1039/d1qi00065a ◽

2021 ◽

Author(s):

Yingchun Zhang ◽

Changsheng Cao ◽

Xintao Wu ◽

Qi-Long Zhu

Keyword(s):

Current Density ◽

High Current Density ◽

Three Dimensional ◽

Co2 Reduction ◽

Reduction Reaction ◽

High Current ◽

Porous Copper ◽

Reduction Of Co2 ◽

Co2 Reduction Reaction ◽

Wide Potential

Bismuth (Bi)-based nanomaterials are considered as the promising electrocatalysts for electrocatalytic CO2 reduction reaction (CO2RR), but it is challenging to achieve high current density and selectivity in a wide potential...

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Quasi-graphitic carbon shell-induced Cu confinement promotes electrocatalytic CO2 reduction toward C2+ products

Nature Communications ◽

10.1038/s41467-021-24105-9 ◽

2021 ◽

Vol 12 (1) ◽

Author(s):

Ji-Yong Kim ◽

Deokgi Hong ◽

Jae-Chan Lee ◽

Hyoung Gyun Kim ◽

Sungwoo Lee ◽

...

Keyword(s):

High Efficiency ◽

Co2 Reduction ◽

Value Added ◽

Material Design ◽

Catalyst System ◽

Critical Issue ◽

Reduction Reaction ◽

Catalyst Design ◽

Design Strategies ◽

Faradaic Efficiency

AbstractFor steady electroconversion to value-added chemical products with high efficiency, electrocatalyst reconstruction during electrochemical reactions is a critical issue in catalyst design strategies. Here, we report a reconstruction-immunized catalyst system in which Cu nanoparticles are protected by a quasi-graphitic C shell. This C shell epitaxially grew on Cu with quasi-graphitic bonding via a gas–solid reaction governed by the CO (g) - CO2 (g) - C (s) equilibrium. The quasi-graphitic C shell-coated Cu was stable during the CO2 reduction reaction and provided a platform for rational material design. C2+ product selectivity could be additionally improved by doping p-block elements. These elements modulated the electronic structure of the Cu surface and its binding properties, which can affect the intermediate binding and CO dimerization barrier. B-modified Cu attained a 68.1% Faradaic efficiency for C2H4 at −0.55 V (vs RHE) and a C2H4 cathodic power conversion efficiency of 44.0%. In the case of N-modified Cu, an improved C2+ selectivity of 82.3% at a partial current density of 329.2 mA/cm2 was acquired. Quasi-graphitic C shells, which enable surface stabilization and inner element doping, can realize stable CO2-to-C2H4 conversion over 180 h and allow practical application of electrocatalysts for renewable energy conversion.

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Hierarchical three-dimensional copper selenide nanocubes microelectrodes for improved carbon dioxide reduction reaction

Sustainable Energy & Fuels ◽

10.1039/d1se01458g ◽

2021 ◽

Author(s):

Rajasekaran Elakkiya ◽

Govindhan Maduraiveeran

Keyword(s):

Carbon Dioxide ◽

High Performance ◽

Three Dimensional ◽

Co2 Reduction ◽

Value Added ◽

Carbon Dioxide Reduction ◽

Reduction Reaction ◽

Earth Abundant ◽

Carbon Dioxide Co2 ◽

Co2 Reduction Reaction

Design of high-performance and Earth-abundant electrocatalysts for electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) into fuels and value-added chemicals offers an emergent pathway for environment and energy sustainable concerns. Herein,...

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Graphene Supported Tungsten Carbide as Catalyst for Electrochemical Reduction of CO2

Catalysts ◽

10.3390/catal9070604 ◽

2019 ◽

Vol 9 (7) ◽

pp. 604

Author(s):

Sahithi Ananthaneni ◽

Zachery Smith ◽

Rees B. Rankin

Keyword(s):

Tungsten Carbide ◽

Electrochemical Reduction ◽

Density Functional ◽

Low Cost ◽

Co2 Reduction ◽

Platinum Group Metal ◽

Reduction Reaction ◽

Depth Study ◽

Reduction Of Co2 ◽

Co2 Reduction Reaction

Electrochemical reduction of CO2 to useful chemical and fuels in an energy efficient way is currently an expensive and inefficient process. Recently, low-cost transition metal-carbides (TMCs) have been proven to exhibit similar electronic structure similarities to Platinum-Group-Metal (PGM) catalysts and hence, can be good substitutes for some important reduction reactions. In this work, we test graphene-supported WC (Tungsten Carbide) nanoclusters as an electrocatalyst for the CO2 reduction reaction. Specifically, we perform density functional theory (DFT) studies to understand various possible reaction mechanisms and determine the lowest thermodynamic energy landscape of CO2 reduction to various products, such as CO, HCOOH, CH3OH, and CH4. This in-depth study of reaction energetics could lead to improvements and development of more efficient electrocatalysts for CO2 reduction.

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Optimizing the use of a “Zero-Gap” Gas Diffusion Electrode Setup for Electrochemical Reduction of CO2

10.26434/chemrxiv-2021-8k376 ◽

2021 ◽

Author(s):

Shima Alinejad ◽

Jonathan Quinson ◽

Yao Li ◽

Ying Kong ◽

Sven Reichenberger ◽

...

Keyword(s):

Co2 Reduction ◽

Catalyst Layer ◽

Gas Diffusion ◽

Reduction Reaction ◽

Gas Diffusion Electrode ◽

Test Bed ◽

Catalyst Screening ◽

Electrochemical Co2 Reduction ◽

Reduction Of Co2 ◽

Co2 Reduction Reaction

The lack of a robust and standardized experimental test bed to investigate the performance of catalyst materials for the electrochemical CO2 reduction reaction (ECO2RR) is one of the major challenges in this field of research. To best reproduce and mimic commercially relevant conditions for catalyst screening and testing, gas diffusion electrode (GDE) setups attract a rising attention as an alternative to conventional aqueous-based setups such as the H-cell configuration. In particular a zero-gap design shows promising features for upscaling to the commercial scale. In this study, we develop further our recently introduced zero-gap GDE setup for the CO2RR using an Au electrocatalyst as model system and identify/report the key experimental parameters to control in the catalyst layer preparation in order to optimize the activity and selectivity of the catalyst.

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Photoelectrochemical Reduction of CO2 to Syngas by Reduced Ag Catalysts on Si Photocathodes

Applied Sciences ◽

10.3390/app10103487 ◽

2020 ◽

Vol 10 (10) ◽

pp. 3487 ◽

Cited By ~ 1

Author(s):

Changyeon Kim ◽

Seokhoon Choi ◽

Min-Ju Choi ◽

Sol A Lee ◽

Sang Hyun Ahn ◽

...

Keyword(s):

Catalytic Activity ◽

Active Sites ◽

Co2 Reduction ◽

Reduction Reaction ◽

Hydrogen Electrode ◽

Faradaic Efficiency ◽

Onset Potential ◽

Reduction Of Co2 ◽

Co2 Reduction Reaction ◽

Ag Catalysts

The photoelectrochemical reduction of CO2 to syngas that is used for many practical applications has been emerging as a promising technique to relieve the increase of CO2 in the atmosphere. Si has been considered to be one of the most promising materials for photoelectrodes, but the integration of electrocatalysts is essential for the photoelectrochemical reduction of CO2 using Si. We report an enhancement of catalytic activity for CO2 reduction reaction by Ag catalysts of tuned morphology, active sites, and electronic structure through reducing anodic treatment. Our proposed photocathode structure, a SiO2 patterned p-Si photocathode with these reduced Ag catalysts, that was fabricated using electron-beam deposition and electrodeposition methods, provides a low onset-potential of −0.16 V vs. the reversible hydrogen electrode (RHE), a large saturated photocurrent density of −9 mA/cm2 at −1.23 V vs. RHE, and faradaic efficiency for CO of 47% at −0.6 V vs. RHE. This photocathode can produce syngas in the ratio from 1:1 to 1:3, which is an appropriate proportion for practical application. This work presents a new approach for designing photocathodes with a balanced catalytic activity and light absorption to improve the photoelectrochemical application for not only CO2 reduction reaction, but also water splitting or N2 reduction reaction.

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Engineering conductive network of atomically thin bismuthene with rich defects enables CO2 reduction to formate with industry-compatible current densities and stability

Energy & Environmental Science ◽

10.1039/d1ee01495a ◽

2021 ◽

Author(s):

Min Zhang ◽

Wenbo Wei ◽

Shenghua Zhou ◽

Dong-Dong Ma ◽

Aihui Cao ◽

...

Keyword(s):

Co2 Reduction ◽

Value Added ◽

Reduction Reaction ◽

Conductive Network ◽

Electrochemical Co2 Reduction ◽

Liquid Products ◽

Current Densities ◽

Co2 Reduction Reaction

Electrochemical CO2 reduction reaction (CO2RR) to value-added and readily collectable liquid products is promising but remains a great challenge due to the lack of efficient and robust electrocatalysts. Herein, a...

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