scholarly journals Through-Space Electronic Conjugation Enhances Co-Electrocatalytic Reduction of CO2 to CO by a Molecular Cr Complex

Author(s):  
Shelby L. Hooe ◽  
Juan Moreno ◽  
Amelia Reid ◽  
Emma Cook ◽  
Charles Machan

The electrocatalytic reduction of CO2 represents an appealing method for converting renewable energy sources into value-added chemical feedstocks. Here, we report a co-electrocatalytic system for the reduction of CO2 to CO comprised of a molecular Cr complex, Cr(tbudhbpy)Cl(H2O) 1, where 6,6′-di(3,5-di-tert-butyl- 2-phenolate)-2,2′-bipyridine = [tbudhbpy]2- and dibenzothiophene-5,5-dioxide (DBTD) as a redox mediator which achieves high activity (1.51-2.84 x 105 s–1) and quantitative selectivity. Under aprotic or protic conditions, DBTD produces a co-electrocatalytic response with 1 by coordinating trans to the site of CO2 binding and mediating electron transfer from the electrode with quantitative efficiency for CO. This assembly is in part reliant on through-space electronic conjugation between the π frameworks of DBTD and the bpy fragment of the catalyst ligand, with important contributions from dispersion interactions and weak sulfone coordination to Cr. Experimental and computational results suggest that this interaction stabilizes a key intermediate in a new aprotic catalytic pathway and lowers the rate-determining transition state under protic conditions. To the best of our knowledge through-space electronic conjugation has not been explored in molecular electrocatalytic systems.<br>

2021 ◽  
Author(s):  
Shelby L. Hooe ◽  
Juan Moreno ◽  
Amelia Reid ◽  
Emma Cook ◽  
Charles Machan

The electrocatalytic reduction of CO2 represents an appealing method for converting renewable energy sources into value-added chemical feedstocks. Here, we report a co-electrocatalytic system for the reduction of CO2 to CO comprised of a molecular Cr complex, Cr(tbudhbpy)Cl(H2O) 1, where 6,6′-di(3,5-di-tert-butyl- 2-phenolate)-2,2′-bipyridine = [tbudhbpy]2- and dibenzothiophene-5,5-dioxide (DBTD) as a redox mediator which achieves high activity (1.51-2.84 x 105 s–1) and quantitative selectivity. Under aprotic or protic conditions, DBTD produces a co-electrocatalytic response with 1 by coordinating trans to the site of CO2 binding and mediating electron transfer from the electrode with quantitative efficiency for CO. This assembly is in part reliant on through-space electronic conjugation between the π frameworks of DBTD and the bpy fragment of the catalyst ligand, with important contributions from dispersion interactions and weak sulfone coordination to Cr. Experimental and computational results suggest that this interaction stabilizes a key intermediate in a new aprotic catalytic pathway and lowers the rate-determining transition state under protic conditions. To the best of our knowledge through-space electronic conjugation has not been explored in molecular electrocatalytic systems.<br>


2021 ◽  
Author(s):  
Shelby L. Hooe ◽  
Juan Moreno ◽  
Amelia Reid ◽  
Emma Cook ◽  
Charles Machan

The electrocatalytic reduction of CO<sub>2</sub> is an appealing method for converting renewable energy sources into value-added chemical feedstocks. We report a co-electrocatalytic system for the reduction of CO<sub>2</sub> to CO comprised of a molecular Cr complex and dibenzothiophene-5,5-dioxide (DBTD) as a redox mediator which achieves high activity (TOF = 1.51-2.84 x 10<sup>5</sup> s<sup>–1</sup>) and quantitative selectivity. Under aprotic or protic conditions, DBTD produces a co-electrocatalytic response with <b>1</b> by coordinating <i>trans</i> to the site of CO<sub>2</sub> binding and mediating electron transfer from the electrode with quantitative efficiency for CO. This assembly is reliant on through-space electronic conjugation between the <i>π</i> frameworks of DBTD and the bpy fragment of the catalyst ligand, with contributions from dispersive interactions and weak sulfone coordination. The resulting interaction stabilizes a key intermediate in a new aprotic catalytic pathway and lowers the energy of the rate-determining transition state under protic conditions. To the best of our knowledge through-space electronic conjugation has not been explored in molecular electrocatalytic systems.<br>


2017 ◽  
Vol 19 (10) ◽  
pp. 2406-2415 ◽  
Author(s):  
Chiara Genovese ◽  
Claudio Ampelli ◽  
Siglinda Perathoner ◽  
Gabriele Centi

A study on the mechanism of C–C bond formation in the electrocatalytic reduction of CO2 to acetic acid with Cu/CNT electrocatalysts.


Energies ◽  
2021 ◽  
Vol 14 (24) ◽  
pp. 8537
Author(s):  
Dimitrios Stamopoulos ◽  
Petros Dimas ◽  
Ioannis Sebos ◽  
Aggelos Tsakanikas

As more economies are transitioning away from fossil fuels for their electricity production and towards greener alternatives, many socioeconomic implications of this shift remain actively debated. The present paper attempts to assess the economic impact of investments in renewable energy sources (RESs) for Greece and whether the broader effects of this transition can offset the negative impact that will occur due to the targeted phase-out of lignite plants by 2028, which constitute the predominant power source for Greece. Our methodological approach builds on input–output analysis and the creation of composite RES industries for the estimation of the net effects of a series of monetary shocks that correspond to Greece’s phase-out investment plan, utilizing the most recent national input–output tables and satellite structural business statistics. We focus on the structural effects of these shocks on a series of socioeconomic indicators, including GDP, employment, wages, government income (through taxes), and capital formation. The results indicate that even though lignite power production still provides a significant contribution to the Greek economy, investing in renewables presents a significant opportunity for value added and job creation.


2020 ◽  
Vol 8 (19) ◽  
pp. 9776-9787 ◽  
Author(s):  
Xurui Zhang ◽  
Yanxing Zhang ◽  
Qingqing Li ◽  
Xiaodong Zhou ◽  
Qingyu Li ◽  
...  

Electrochemical reduction of carbon dioxide (ERCO2) to low-carbon fuel and useful chemicals, which can simultaneously store renewable energy and recover CO2 in a green manner, has proven to be a viable energy storage and conversion strategy.


Author(s):  
M. D. Simonova ◽  
V. E. Zakharov

The article focuses on the economic and statistical analysis of industries associated with the use of renewable energy sources in several countries. The dynamic development and implementation of technologies based on renewable energy sources (hereinafter RES) is the defining trend of world energy development. The uneven distribution of hydrocarbon reserves, increasing demand of developing countries and environmental risks associated with the production and consumption of fossil resources has led to an increasing interest of many states to this field. Creating low-carbon economies involves the implementation of plans to increase the proportion of clean energy through renewable energy sources, energy efficiency, reduce greenhouse gas emissions. The priority of this sector is a characteristic feature of modern development of developed (USA, EU, Japan) and emerging economies (China, India, Brazil, etc.), as evidenced by the inclusion of the development of this segment in the state energy strategies and the revision of existing approaches to energy security. The analysis of the use of renewable energy, its contribution to value added of countries-producers is of a particular interest. Over the last decade, the share of energy produced from renewable sources in the energy balances of the world's largest economies increased significantly. Every year the number of power generating capacity based on renewable energy is growing, especially, this trend is apparent in China, USA and European Union countries. There is a significant increase in direct investment in renewable energy. The total investment over the past ten years increased by 5.6 times. The most rapidly developing kinds are solar energy and wind power.


Energies ◽  
2021 ◽  
Vol 15 (1) ◽  
pp. 2
Author(s):  
Davor Mikulić ◽  
Damira Keček

Croatian energy strategy defines ambitious goals aimed at achieving energy transition toward a sustainable low-carbon society. Achieving those goals requires significant investments in the renewable energy sources and improved energy efficiency of buildings. The purpose of this paper is to estimate and compare the economic effects of the energy transition on the renewable energy supply and demand side. The estimation of the energy transition effects in Croatia in the period 2020–2050 is based on the input-output model, which identifies direct, indirect and induced effects of investments in renewable energy sources and energy efficient buildings renovation. Results of the study reveal relatively higher gross value added and employment effects induced by investments in building retrofits, but the effects of investments in renewable energy are also significant. Investments in sustainable, efficient and environmentally effective energy system could significantly contribute to Croatian GDP. While GVA effects range from 0.4% to 0.6% of annual GDP, the share of full-time equivalent jobs induced by energy transition could reach 0.5% to 1% of total employment in Croatia. Investments in RES plants and energy efficient building reconstruction are not substitutes but complements which ensure a smooth energy transition if undertaken together.


IEE Review ◽  
1991 ◽  
Vol 37 (4) ◽  
pp. 152
Author(s):  
Kenneth Spring

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