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33. Triggering C‒N Coupling on Metal Oxide Nanocomposite for the Electrochemical Reduction of CO2 and NOx⁻ to Formamide.

Author

Ramadhany, Putri, Trần‐Phú, Thành, Yuwono, Jodie A., Ma, Zhipeng, Han, Chen, Nguyen, Thi Kim Anh, Leverett, Josh, Kumar, Priyank, Hocking, Rosalie K., Tricoli, Antonio, Simonov, Alexandr N., Amal, Rose, and Daiyan, Rahman

Abstract

The co‐electroreduction of CO2 and NOx⁻ (NO3⁻/NO2⁻) to generate formamide (HCONH2) offers an opportunity for downstream chemical and polymer manufacturing decarbonization; however, significant challenges lie in the C‒N coupling and the associated low product selectivity. Herein, p‐block metal oxides are incorporated in copper oxides to provide more accessible active sites for reactant adsorption and activation, tuning the reaction selectivity toward the formamide production. Through in situ Raman and synchrotron‐based infrared spectroscopy measurements, C─N bond formation is demonstrated in real‐time with the CuOx/BiOx catalyst, where the C─N bond is detected via a *CHO and *NH2 intermediates formation, in agreement with the density functional theory calculations. When tested in a flow electrolyzer, a formamide yield rate of 134 ± 11 mmol h−1 gcat−1 is reported, the first report of co‐electroreduction of CO2 and NOx⁻ to formamide beyond conventional H‐cell measurements. These new insights on the C‒N coupling mechanisms and scale‐up capability provide directions for further development of electrocatalysts for the formamide production. [ABSTRACT FROM AUTHOR]

Published
2024
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36. From Plastic Waste to Green Hydrogen and Valuable Chemicals Using Sunlight and Water.

Author

Anh Nguyen, Thi Kim, Trần‐Phú, Thành, Daiyan, Rahman, Minh Chau Ta, Xuan, Amal, Rose, and Tricoli, Antonio

Abstract

Over 79 % of 6.3 billion tonnes of plastics produced from 1950 to 2015 have been disposed in landfills or found their way to the oceans, where they will reside for up to hundreds of years before being decomposed bringing upon significant dangers to our health and ecosystems. Plastic photoreforming offers an appealing alternative by using solar energy and water to transform plastic waste into value‐added chemical commodities, while simultaneously producing green hydrogen via the hydrogen evolution reaction. This review aims to provide an overview of the underlying principles of emerging plastic photoreforming technologies, highlight the challenges associated with experimental protocols and performance assessments, discuss recent global breakthroughs on the photoreforming of plastics, and propose perspectives for future research. A critical assessment of current plastic photoreforming studies shows a lack of standardised conditions, hindering comparison amongst photocatalyst performance. Guidelines to establish a more accurate evaluation of materials and systems are proposed, with the aim to facilitate the translation of promising fundamental discovery in photocatalysts design. [ABSTRACT FROM AUTHOR]

Published
2024
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38. Rationally Designed Carbon‐Based Catalysts for Electrochemical C‐N Coupling.

Author

Li, Yan, Verma, Vandana, Su, Hongli, Zhang, Xiaoran, Zhou, Shujie, Lawson, Tom, Li, Jingliang, Amal, Rose, Hou, Yang, and Dai, Liming

Subjects
ELECTROSYNTHESIS, NITROGEN compounds, ELECTROLYTIC reduction, BOND formation mechanism, NITRITES, CATALYSTS, CARBON dioxide reduction, CARBON offsetting, NITROGEN cycle
Abstract

The electrochemical C‐N coupling process, facilitating the production of organic nitrogen substances (such as urea, methylamine, formamide, and ethylamine) via the simultaneous reduction of carbon dioxide (CO2) and small nitrogen‐based substances, stands at the forefront of advancing carbon neutrality and the artificial nitrogen cycle. This method has garnered substantial interest due to its potential economic and environmental benefits. Although considerable progress has been achieved in this emerging field, it still faces challenges, including slow reactant adsorption, competing side reactions, and complex multi‐step pathways, resulting in low yields and selectivity. Strategically designing and developing low‐cost and exceptionally performant catalysts is crucial for cost‐effective and precise electrochemical C─N bonding. This article offers an in‐depth review of the electrosynthesis of valuable organic nitrogen compounds at ambient conditions from earth‐abundant resources/wastes, such as CO2 and small nitrogenous molecules (nitrogen: N2, nitrite: NO2−, nitrate: NO3−, ammonia: NH3, etc.), via electrochemical C─N bond formation reactions, especially using carbon‐based catalysts. The relevant electrochemical C─N bond formation mechanisms, the design principles of advanced carbon‐based electrocatalysts, and the impact of different electrolyser designs are discussed, along with the present obstacles and upcoming prospects in this dynamic field. [ABSTRACT FROM AUTHOR]

Published
2024
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