Dual-Doped Nickel Sulfide for Electro-Upgrading Polyethylene Terephthalate into Valuable Chemicals and Hydrogen Fuel

IF 31.6 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Nano-Micro Letters Pub Date : 2023-09-11 DOI:10.1007/s40820-023-01181-8

Zhijie Chen, Renji Zheng, Teng Bao, Tianyi Ma, Wei Wei, Yansong Shen, Bing-Jie Ni

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Abstract

Electro-upcycling of plastic waste into value-added chemicals/fuels is an attractive and sustainable way for plastic waste management. Recently, electrocatalytically converting polyethylene terephthalate (PET) into formate and hydrogen has aroused great interest, while developing low-cost catalysts with high efficiency and selectivity for the central ethylene glycol (PET monomer) oxidation reaction (EGOR) remains a challenge. Herein, a high-performance nickel sulfide catalyst for plastic waste electro-upcycling is designed by a cobalt and chloride co-doping strategy. Benefiting from the interconnected ultrathin nanosheet architecture, dual dopants induced up-shifting d band centre and facilitated in situ structural reconstruction, the Co and Cl co-doped Ni₃S₂ (Co, Cl-NiS) outperforms the single-doped and undoped analogues for EGOR. The self-evolved sulfide@oxyhydroxide heterostructure catalyzes EG-to-formate conversion with high Faradic efficiency (> 92%) and selectivity (> 91%) at high current densities (> 400 mA cm⁻²). Besides producing formate, the bifunctional Co, Cl-NiS-assisted PET hydrolysate electrolyzer can achieve a high hydrogen production rate of 50.26 mmol h⁻¹ in 2 M KOH, at 1.7 V. This study not only demonstrates a dual-doping strategy to engineer cost-effective bifunctional catalysts for electrochemical conversion processes, but also provides a green and sustainable way for plastic waste upcycling and simultaneous energy-saving hydrogen production.

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双掺杂硫化镍电升级聚对苯二甲酸乙二醇酯为有价化学品和氢燃料。

电子升级回收塑料废物为增值化学品/燃料是塑料废物管理的一种有吸引力和可持续的方式。近年来，电催化将聚对苯二甲酸乙二醇酯(PET)转化为甲酸酯和氢引起了人们的极大兴趣，但开发高效、低成本、高选择性的中心乙二醇(PET单体)氧化反应催化剂仍然是一个挑战。本文采用钴和氯化物共掺杂策略，设计了一种用于塑料垃圾电升级回收的高性能硫化镍催化剂。Co和Cl共掺Ni3S2 (Co, Cl- nis)的EGOR性能优于单掺杂和未掺杂的类似物，得益于相互连接的超薄纳米片结构，双掺杂诱导d带中心上移并促进原位结构重建。在高电流密度(> 400 mA cm-2)下，自进化的sulfide@oxyhydroxide异质结构具有高的Faradic效率(> 92%)和选择性(> 91%)。除产甲酸外，双官能团Co, cl - ni辅助的PET水解产物电解槽在2 M KOH、1.7 V条件下的产氢率可达50.26 mmol h-1。该研究不仅展示了双掺杂策略，为电化学转化过程设计具有成本效益的双功能催化剂，而且为塑料废物升级回收和同时节能制氢提供了绿色可持续的途径。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano-Micro Letters NANOSCIENCE & NANOTECHNOLOGY-MATERIALS SCIENCE, MULTIDISCIPLINARY

CiteScore

42.40

自引率

4.90%

发文量

715

审稿时长

13 weeks

期刊介绍： Nano-Micro Letters is a peer-reviewed, international, interdisciplinary and open-access journal that focus on science, experiments, engineering, technologies and applications of nano- or microscale structure and system in physics, chemistry, biology, material science, pharmacy and their expanding interfaces with at least one dimension ranging from a few sub-nanometers to a few hundreds of micrometers. Especially, emphasize the bottom-up approach in the length scale from nano to micro since the key for nanotechnology to reach industrial applications is to assemble, to modify, and to control nanostructure in micro scale. The aim is to provide a publishing platform crossing the boundaries, from nano to micro, and from science to technologies.