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Metal graphdiyne towards electrochemical water splitting

Periodic Reporting for period 1 - CarbonChem (Metal graphdiyne towards electrochemical water splitting)

Okres sprawozdawczy: 2022-01-26 do 2024-01-25

‘Green Hydrogen (H2)’ is an ideal clean energy source, due to high calorific value, which is considered as alternative to instead of traditional fossil fuels. European commission has initiated the ‘Clean Hydrogen Alliance’ and launched a new ‘European Industrial Strategy’ for promoting the development of the hydrogen industry. To date, steam methane reforming is the main method for hydrogen production (over 94% in Europe), which is operated under harsh conditions and is energy intensive. Electrochemical water splitting is an ultimate strategy with environmentally-friend and low-consumption, which involves two half-reactions: hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Owing to the sluggish kinetics of HER and OER, electrocatalyst is intensely desired to reduce their overpotentials and facilitate practical applications.
It is known that the current scope of electrocatalysts utilized for water splitting reactions is dominated by inorganic nanomaterials, their metal active sites only exist on the surface and/or edge of the nanostructures. The major unexposed metal atoms in the bulk phase are inert for electrocatalysis, which strictly limits the metal atom utilization. In particular, because of the fixed crystal structure, the current inorganic nanomaterials are difficult to continue as proper models to reveal mechanism of high-efficiency single-atom electrocatalysis, that encumbers the development of electrocatalytic technologies. In order to break this bottleneck, the proposed research project aims at re-defining the concept of electrocatalysts and will achieve a new-type scientific platform for single-atom electrocatalysis of water splitting.
Inspired by single-atom electrocatalysts, the project integrated covalent-organic frameworks and graphdiyne, achieved a novel conductive metal covalent-organic frameworks (MCOFs) catalyst toward water splitting. The new MCOFs increased the metal content of SACs to ~ 2 at%, which is much higher than that of traditional SCAs (≤ 1 at%), the abundant active metal centers will bring a huge improvement of electrocatalytic performance for MCOFs. Moreover, by engineering chemical composition, a series of MCOFs with different metal center was synthesized. The corresponding physical properties (chemical structure, optical and electrical properties) were investigated by various technologies, including scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), infrared spectrometer and UV absorption spectrum. Additionally, the electrochemical investigation displayed that the new MCOFs with high metal content has a good HER behavior.
In order to reveal the catalytic mechanism of SACs, the ER cooperated with several well-known research groups worldwide. By starting with traditional inorganic nanocatalysts, the catalytic mechanism of SACs toward water splitting has been gradually clarified. That laid the foundation of establishing a mechanism platform toward SCAs catalysis, which will re-defining the concept of next-generation electrocatalysts. The mechanism platform will contribute to the development of hydrogen and other electrochemical industries.
The project has developed new know-how and knowledge in the areas of i) single-atom electrocatalysts, ii) water splitting and iii) electrocatalytic mechanism.
Metal covalent-organic frameworks (MCOFs) is a type of advanced single-atom electrocatalysts (SACs), which not only have controllable chemical structure, but possess more abundant active metal center rather than current SACs (metal content ≤ 1 at%). Besides, only few MCOFs was utilized toward electrochemical reaction, especially hydrogen production.
The project will achieve a novel MCOFs with ultra-high metal content (≥ 14 at%), that is almost close to traditional inorganic catalysts. The ultra-high active metal centers will achieve an outstanding electrocatalytic property for the novel MCOFs. Thus, the project will bring a technological revolution for European hydrogen industry: (1) increasing the practicability of electrochemical hydrogen production, that will reduce environmental pollution during hydrogen production; (2) decreasing energy consumption in hydrogen industry.
On the other hand, the investigation of electrocatalytic mechanism in the project will reveal the catalytic principle of SACs, and establish a new platform to further understand electrocatalytic process. The project will propose a new design concept of next-generation electrocatalytic materials for hydrogen production and other energy and environment industries, including carbon conversion, nitrogen fixation and metal-air battery etc.
Graphic abstract for ‘CarbonChem’ project
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