Synthesis and Catalytic Performance of Metal–Organic Framework-Derived Porous Carbon Nanostructures for Electrocatalytic CO2 Reduction and Oxygen Evolution Reactions

Project Abstract

We report a comprehensive study on the synthesis, characterization, and catalytic evaluation of metal–organic framework (MOF)-derived porous carbon nanostructures as electrocatalysts for CO2 reduction reactions (CO2RR) and oxygen evolution reactions (OER). A robust synthesis strategy was developed to convert a single, readily available MOF precursor into hierarchical carbon networks with tunable porosity, high surface area, and embedded transition metal–nitrogen active sites. The process involves controlled pyrolysis under inert atmosphere followed by selective activation and, where appropriate, post-synthetic heteroatom doping to tailor electronic structure and catalytic sites. Detailed material characterization by X-ray diffraction, Raman spectroscopy, transmission and scanning electron microscopy, N2 adsorption–desorption isotherms, X-ray photoelectron spectroscopy, and inductively coupled plasma mass spectrometry confirms the formation of interconnected graphitic domains interspersed with micro- and mesopores, promoting efficient mass transport and high active site density. Electrochemical evaluation was performed in aqueous electrolyte under ambient conditions using a standard three-electrode configuration. For CO2RR, the catalysts demonstrate a high Faradaic efficiency toward CO and formate across a wide potential window, with suppressed hydrogen evolution due to optimized binding energies of key intermediates on N-doped carbon and metal–nitrogen–carbon motifs derived from the MOF scaffold. The observed onset potentials and Tafel slopes indicate rapid electron transfer and favorable reaction kinetics, supported by operando spectroscopy that reveals dynamic restructuring of active sites under catalytic bias. For OER, the MOF-derived porous carbon exhibits low overpotentials and high current densities, attributed to synergetic effects between graphitic carbon support and electroactive Fe–N or Co–N moieties, which facilitate water oxidation through low-lying O–OH intermediate formation and efficient charge transfer. Density functional theory calculations complement the experimental findings by elucidating adsorption energetics and reaction pathways, showing that pore architecture and heteroatom doping modulate the adsorption free energies of *COOH, *CO, and *OH intermediates, thereby tuning selectivity and activity. A coupled experimental–theoretical framework demonstrates the stability of active sites over prolonged operation, with minimal structural degradation and sustained catalytic performance over 50+ hours of continuous operation. The study further investigates electrochemical surface area normalization, electrolyte effects, and catalyst loading to optimize scalability and real-world applicability. Life cycle considerations discuss the environmental and economic implications of MOF-derived materials, highlighting their potential to replace scarce precious-metal catalysts in CO2 utilization and renewable energy storage technologies. Overall, the work provides a versatile, scalable route to engineer MOF-derived porous carbon nanostructures with tailored active sites, enabling high-efficiency, selective electrocatalysis for CO2 reduction and water oxidation.

Project Overview

What This Project Is About

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This project explores creating porous carbon materials from metal–organic frameworks (MOFs) and testing their ability to help two key chemical processes: converting carbon dioxide (CO2) into useful chemicals and water splitting to release oxygen. The idea is to turn a MOF into a carbon-based catalyst with many tiny pores, which can boost reactions while using less energy and producing fewer unwanted byproducts.

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The Problem It Addresses

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Currently, efficient, affordable catalysts for CO2 reduction and oxygen evolution are hard to find. Many materials perform well in one reaction but not both, or they require expensive metals. This project aims to create a versatile, cost-effective material that works well for both reactions, helping reduce greenhouse gases and improve renewable energy technologies.

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Objectives of the Project

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1. Understand how MOFs can be transformed into porous carbon catalysts.
2. Characterize the structure and porosity of the derived carbon materials.
3. Evaluate catalytic performance for CO2 reduction and oxygen evolution reactions (OER).
4. Identify the best material composition and treatment conditions for dual functionality.
5. Assess stability and reusability of the catalysts under reaction conditions.

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What You Will Do Step by Step

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1. Synthesize a MOF and prepare carbonized products with controlled porosity. 2. Characterize materials using basic techniques (surface area, pore size, and composition). 3. Set up simple electrochemical tests to measure CO2 reduction activity and OER activity. 4. Compare performance across different carbon structures. 5. Analyze data to link structure with activity. 6. Test durability by repeated reaction cycles. 7. Summarize findings and propose practical improvements. 8. Discuss potential environmental and energy implications.

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Expected Outcome

The project should produce a well-characterized MOF-derived porous carbon catalyst with demonstrated activity for both CO2 reduction and OER, plus insights into how pore structure and composition affect performance. It should offer practical guidance for material design in sustainable chemistry and energy applications.