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A universal and scalable transformation of bulk metals into single-atom catalysts in ionic liquids.

ABSTRACT: Single-atom catalysts (SACs) with maximized metal atom utilization and intriguing properties are of utmost importance for energy conversion and catalysis science. However, the lack of a straightforward and scalable synthesis strategy of SACs on diverse support materials remains the bottleneck for their large-scale industrial applications. Herein, we report a general approach to directly transform bulk metals into single atoms through the precise control of the electrodissolution-electrodeposition kinetics in ionic liquids and demonstrate the successful applicability of up to twenty different monometallic SACs and one multimetallic SAC with five distinct elements. As a case study, the atomically dispersed Pt was electrodeposited onto Ni₃N/Ni-Co-graphene oxide heterostructures in varied scales (up to 5 cm × 5 cm) as bifunctional catalysts with the electronic metal-support interaction, which exhibits low overpotentials at 10 mA cm^-2 for hydrogen evolution reaction (HER, 30 mV) and oxygen evolution reaction (OER, 263 mV) with a relatively low Pt loading (0.98 wt%). This work provides a simple and practical route for large-scale synthesis of various SACs with favorable catalytic properties on diversified supports using alternative ionic liquids and inspires the methodology on precise synthesis of multimetallic single-atom materials with tunable compositions.

SUBMITTER: Wang S

PROVIDER: S-EPMC10927526 | biostudies-literature | 2024 Mar

REPOSITORIES: biostudies-literature

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A universal and scalable transformation of bulk metals into single-atom catalysts in ionic liquids.

Wang Shujuan S Lu Minghui M Xia Xuewen X Wang Fei F Xiong Xiaolu X Ding Kai K Pang Zhongya Z Li Guangshi G Xu Qian Q Hsu Hsien-Yi HY Hu Shen S Ji Li L Zhao Yufeng Y Wang Jing J Zou Xingli X Lu Xionggang X

Proceedings of the National Academy of Sciences of the United States of America 20240226 10

Single-atom catalysts (SACs) with maximized metal atom utilization and intriguing properties are of utmost importance for energy conversion and catalysis science. However, the lack of a straightforward and scalable synthesis strategy of SACs on diverse support materials remains the bottleneck for their large-scale industrial applications. Herein, we report a general approach to directly transform bulk metals into single atoms through the precise control of the electrodissolution-electrodepositio ...[more]

PMID: 38408257

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Project description:The escalating issue of plastic waste generation has prompted the search for an effective solution to address these challenges. In this study, we present a novel plasma-enabled strategy for the rapid breakdown of various types of plastic wastes, including mixtures, into high-value carbon nanomaterials and hydrogen. The H2 yield and selectivity achieved through the implemented catalyst-free plasma-enabled strategy are 14.2 and 5.9 times higher, respectively, compared to those obtained with conventional thermal pyrolysis under similar conditions. It is noteworthy that this catalyst-free plasma alone approach yields a significantly higher energy yield of H2 (gH2/kWh) compared to other pyrolysis processes. By coupling plasma pyrolysis with thermal catalytic process, employing of 1 wt . % M/CeO2 (M=Fe, Co, and Ni) atomically dispersed catalysts can further enhance hydrogen production. Specifically, the 1 wt . % Co/CeO2 catalyst demonstrated excellent catalytic performance throughout the 10 cycles of plastic waste decomposition, achieving the highest H2 yield of 46.7 mmol/gplastic (equivalent to 64.4 % of theoretical H2 production) and nearly 100 % hydrogen atom recovery efficiency at the 7th cycle. Notably, the H2 yield achieved over the atomically dispersed Fe on CeO2 surface (1 wt . % Fe/CeO2) in the integrated plasma-thermal catalytic process is comparable to that obtained with Fe particles on CeO2 surface (10 wt . % Fe/CeO2). This outcome, demonstrated with single-atom catalysts, offers a promising avenue for cost-effective and efficient chemical plastic recycling. Through a combination of experimental and computational efforts, we have provided an in-depth understanding of the catalytic mechanisms of the investigated single atom catalysts in the developed plasma-enabled process. This innovative and straightforward approach provides a promising and expedient strategy for continuously converting diverse plastic waste streams, including mixed and contaminated sources, into high-value products conducive to a circular plastic economy.

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A universal and scalable transformation of bulk metals into single-atom catalysts in ionic liquids.

Publications

A universal and scalable transformation of bulk metals into single-atom catalysts in ionic liquids.

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