Template-assisted mechanosynthesis (TAMS) for the production of bifunctional transition metal-based catalysts
Date
2024-07-15
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Abstract
Käesolevas doktoritöös uuriti bifunktsionaalsete siirdemetallipõhiste katalüsaatorite väljatöötamist, kasutades uudset malli abiga mehhanokeemilist sünteesimeetodit (TAMS). Doktoritöö eesmärk oli optimeerida katalüsaatormaterjale tsink-õhk akude jaoks, millel on kõrge energiatihedus, kuid on madal võimsustihedus ja piiratud stabiilsus, mis on tingitud aeglasest hapniku redutseerumisest ja eraldumise reaktsioonidest (ORR/OER). Uurimistöö keskendub koobalti-, raua- ja niklipõhiste katalüsaatorite sünteesimisele ja iseloomustamisele. Kiire pürolüüsiga täiustatud TAMS tasakaalustab ORR-aktiivseid üheaatomi/lämmastiku tsentreid ja OER-aktiivseid nanoosakesi, suurendades oluliselt katalüsaatori jõudlust. Täiustatud TAMS-protokoll annab suurema poorsuse ja parema elektrokeemilise aktiivsusega katalüsaatorid. TAMS-ist saadud katalüsaatorid näitasid paremat bifunktsionaalset ORR/OER aktiivsust ja suuremat eripinda, parandades aktiivsete tsentrite juurdepääsetavust ja katalüütilist efektiivsust. Materjalid edestasid kaubanduslikke plaatinarühma metallkatalüsaatoreid oma võimsustiheduse ja tsink-õhk akude pikaajalise stabiilsuse poolest. Väljatöötatud TAMS-i metoodika on säästlikum ja kulutõhusam, nõudes vähem energiat ja aega ilma mürgiseid jäätmeid tekitamata. See doktoritöö edendab elektrokeemilise energia salvestamise valdkonda, pakkudes meetodit suure jõudlusega ja jätkusuutlike katalüsaatorite tootmiseks metall-õhk akude jaoks.
This PhD thesis explores the development of bifunctional transition metal-based catalysts using a novel synthesis method, Template-Assisted Mechanosynthesis (TAMS). The study aims to optimise these catalysts for zinc-air batteries, which have high energy density but struggle with the low power density and limited stability due to slow oxygen reduction and evolution reactions. The research focuses on synthesising and characterising cobalt, iron, and nickel-based catalysts. Enhanced by rapid pyrolysis, TAMS balances ORR-active single-atom/nitrogen sites and OER-active nanoparticles, significantly boosting catalyst performance. The improved TAMS protocol yields catalysts with higher porosity and better electrochemical activity. TAMS-derived catalysts demonstrated superior bifunctional ORR/OER activity and a greater surface area, improving active site accessibility and catalytic efficiency. Materials outperformed commercial platinum group metal catalysts in power density and long-term stability in zinc-air batteries. The developed TAMS methodology is more sustainable and cost-effective, requiring less energy and time without generating toxic waste. This study advances the electrochemical energy storage field by providing a method for producing high-performance, sustainable catalysts for metal-air batteries.
This PhD thesis explores the development of bifunctional transition metal-based catalysts using a novel synthesis method, Template-Assisted Mechanosynthesis (TAMS). The study aims to optimise these catalysts for zinc-air batteries, which have high energy density but struggle with the low power density and limited stability due to slow oxygen reduction and evolution reactions. The research focuses on synthesising and characterising cobalt, iron, and nickel-based catalysts. Enhanced by rapid pyrolysis, TAMS balances ORR-active single-atom/nitrogen sites and OER-active nanoparticles, significantly boosting catalyst performance. The improved TAMS protocol yields catalysts with higher porosity and better electrochemical activity. TAMS-derived catalysts demonstrated superior bifunctional ORR/OER activity and a greater surface area, improving active site accessibility and catalytic efficiency. Materials outperformed commercial platinum group metal catalysts in power density and long-term stability in zinc-air batteries. The developed TAMS methodology is more sustainable and cost-effective, requiring less energy and time without generating toxic waste. This study advances the electrochemical energy storage field by providing a method for producing high-performance, sustainable catalysts for metal-air batteries.
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