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Contact-electro-catalytic CO₂ reduction from ambient air.

ABSTRACT: Traditional catalytic techniques often encounter obstacles in the search for sustainable solutions for converting CO₂ into value-added products because of their high energy consumption and expensive catalysts. Here, we introduce a contact-electro-catalysis approach for CO₂ reduction reaction, achieving a CO Faradaic efficiency of 96.24%. The contact-electro-catalysis is driven by a triboelectric nanogenerator consisting of electrospun polyvinylidene fluoride loaded with single Cu atoms-anchored polymeric carbon nitride (Cu-PCN) catalysts and quaternized cellulose nanofibers (CNF). Mechanistic investigation reveals that the single Cu atoms on Cu-PCN can effectively enrich electrons during contact electrification, facilitating electron transfer upon their contact with CO₂ adsorbed on quaternized CNF. Furthermore, the strong adsorption of CO₂ on quaternized CNF allows efficient CO₂ capture at low concentrations, thus enabling the CO₂ reduction reaction in the ambient air. Compared to the state-of-the-art air-based CO₂ reduction technologies, contact-electro-catalysis achieves a superior CO yield of 33 μmol g^-1 h^-1. This technique provides a solution for reducing airborne CO₂ emissions while advancing chemical sustainability strategy.

SUBMITTER: Wang N

PROVIDER: S-EPMC11246423 | biostudies-literature | 2024 Jul

REPOSITORIES: biostudies-literature

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Contact-electro-catalytic CO2 reduction from ambient air.

Wang Nannan N Jiang Wenbin W Yang Jing J Feng Haisong H Zheng Youbin Y Wang Sheng S Li Bofan B Heng Jerry Zhi Xiong JZX Ong Wai Chung WC Tan Hui Ru HR Zhang Yong-Wei YW Wang Daoai D Ye Enyi E Li Zibiao Z

Nature communications 20240713 1

Traditional catalytic techniques often encounter obstacles in the search for sustainable solutions for converting CO2 into value-added products because of their high energy consumption and expensive catalysts. Here, we introduce a contact-electro-catalysis approach for CO2 reduction reaction, achieving a CO Faradaic efficiency of 96.24%. The contact-electro-catalysis is driven by a triboelectric nanogenerator consisting of electrospun polyvinylidene fluoride loaded with sin ...[more]

PMID: 39003260

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Project description:Due to the dramatically increased atmospheric CO2 concentration and consequential climate change, significant effort has been made to develop sorbents to directly capture CO2 from ambient air (direct air capture, DAC) to achieve negative CO2 emissions in the immediate future. However, most developed sorbents have been studied under a limited array of temperature (>20 °C) and humidity conditions. In particular, the dearth of experimental data on DAC at sub-ambient conditions (e.g., -30 to 20 °C) and under humid conditions will severely hinder the large-scale implementation of DAC because the world has annual average temperatures ranging from -30 to 30 °C depending on the location and essentially no place has a zero absolute humidity. To this end, we suggest that understanding CO2 adsorption from ambient air at sub-ambient temperatures, below 20 °C, is crucial because colder temperatures represent important practical operating conditions and because such temperatures may provide conditions where new sorbent materials or enhanced process performance might be achieved. Here we demonstrate that MIL-101(Cr) materials impregnated with amines (TEPA, tetraethylenepentamine, or PEI, poly(ethylenimine)) offer promising adsorption and desorption behavior under DAC conditions in both the presence and absence of humidity under a wide range of temperatures (-20 to 25 °C). Depending on the amine loading and adsorption temperature, the sorbents show different CO2 capture behavior. With 30 and 50 wt % amine loadings, the sorbents show weak and strong chemisorption-dominant CO2 capture behavior, respectively. Interestingly, at -20 °C, the CO2 adsorption capacity of 30 wt % TEPA-impregnated MIL-101(Cr) significantly increased up to 1.12 mmol/g from 0.39 mmol/g at ambient conditions (25 °C) due to the enhanced weak chemisorption. More importantly, the sorbents also show promising working capacities (0.72 mmol/g) over 15 small temperature swing cycles with an ultralow regeneration temperature (-20 °C sorption to 25 °C desorption). The sub-ambient DAC performance of the sorbents is further enhanced under humid conditions, showing promising and stable CO2 working capacities over multiple humid small temperature swing cycles. These results demonstrate that appropriately designed DAC sorbents can operate in a weak chemisorption modality at low temperatures even in the presence of humidity. Significant energy savings may be realized via the utilization of small temperature swings enabled by this weak chemisorption behavior. This work suggests that significant work on DAC materials that operate at low, sub-ambient temperatures is warranted for possible deployment in temperate and polar climates.

Dataset Information

Contact-electro-catalytic CO₂ reduction from ambient air.

Publications

Contact-electro-catalytic CO<sub>2</sub> reduction from ambient air.

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