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A new operando surface restructuring pathway via ion-pairing of catalyst and electrolyte for water oxidation

Zhuang, Linzhou (author), Li, Zhiheng (author), Li, Mengran (author), Tao, Haolan (author), Mao, Xin (author), Lian, Cheng (author), Ge, Lei (author), Du, Aijun (author), Xu, Zhi (author)

The highly efficient and stable electrolysis needs the rational control of the catalytically active interface during the reactions. Here we report a new operando surface restructuring pathway activated by pairing catalyst and electrolyte ions. Using SrCoO_3-δ-based perovskites as model catalysts, we unveil the critical role of...

journal article 2023

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Electroreduction of Carbon Dioxide to Acetate using Heterogenized Hydrophilic Manganese Porphyrins

Abdinejad, M. (author), Yuan, T. (author), Tang, Keith (author), Duangdangchote, Salatan (author), Iglesias van Montfort, H.P. (author), Li, Mengran (author), Middelkoop, J. (author), Wolff, M.J. (author), Burdyny, T.E. (author)

The electrochemical reduction of carbon dioxide (CO₂) to value-added chemicals is a promising strategy to mitigate climate change. Metalloporphyrins have been used as a promising class of stable and tunable catalysts for the electrochemical reduction reaction of CO₂ (CO₂RR) but have been primarily restricted...

journal article 2023

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Sandwich-like heterostructured nanomaterials immobilized laccase for the degradation of phenolic pollutants and boosted enzyme stability

Li, Mengyu (author), Bai, Yahan (author), Zhuang, Wei (author), Liu, Jinle (author), Wang, Zhi (author), Rao, Yuan (author), Li, Mengran (author), Ying, Hanjie (author), Ouyang, Pingkai (author)

A novel magnetic 2D/2D heterogeneous structure MXene@NiFe-LDH@Fe₃O₄ was prepared for immobilization of laccase. In this work, two-dimensional MXene nanosheets with abundant surface functional groups were heterogeneously assembled with layered double hydroxide (LDH) by in situ co-precipitation method, and magnetic...

journal article 2023

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Non-invasive current collectors for improved current-density distribution during CO₂ electrolysis on super-hydrophobic electrodes

Iglesias van Montfort, H.P. (author), Li, Mengran (author), Irtem, I.E. (author), Abdinejad, M. (author), Wu, Yuming (author), Pal, S.K. (author), Sassenburg, M. (author), Ripepi, D. (author), Subramanian, S.S. (author), Biemolt, J. (author), Rufford, Thomas E. (author), Burdyny, T.E. (author)

Electrochemical reduction of CO₂ presents an attractive way to store renewable energy in chemical bonds in a potentially carbon-neutral way. However, the available electrolyzers suffer from intrinsic problems, like flooding and salt accumulation, that must be overcome to industrialize the technology. To mitigate flooding and salt...

journal article 2023

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An Advanced Guide to Assembly and Operation of CO₂ Electrolyzers

Iglesias van Montfort, H.P. (author), Subramanian, S.S. (author), Irtem, I.E. (author), Sassenburg, M. (author), Li, Mengran (author), Kok, J.J. (author), Middelkoop, J. (author), Burdyny, T.E. (author)

journal article 2023

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High Cationic Dispersity Boosted Oxygen Reduction Reactivity in Multi-Element Doped Perovskites

Li, Wenhuai (author), Li, Mengran (author), Guo, Y. (author), Hu, Zhiwei (author), Zhou, Chuan (author), Brand, Helen E.A. (author), Peterson, Vanessa K. (author), Pao, Chih Wen (author), Chen, Chien Te (author)

Oxygen-ion conducting perovskite oxides are important functional materials for solid oxide fuel cells and oxygen-permeable membranes operating at high temperatures (>500 °C). Co-doped perovskites have recently shown their potential to boost oxygen-related kinetics, but challenges remain in understanding the underlying mechanisms. This...

journal article 2023

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Insertion of MXene-Based Materials into Cu–Pd 3D Aerogels for Electroreduction of CO₂ to Formate

Abdinejad, M. (author), Subramanian, S.S. (author), Motlagh, Mozhgan Khorasani (author), Ripepi, D. (author), Pinto, D. (author), Li, Mengran (author), Middelkoop, J. (author), Urakawa, A. (author), Burdyny, T.E. (author)

The electrochemical CO₂ reduction reaction (CO₂RR) is an attractive method to produce renewable fuel and chemical feedstock using clean energy sources. Formate production represents one of the most economical target products from CO₂RR but is primarily produced using post-transition metal catalysts that...

journal article 2023

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Effect of Dispersing Solvents for an Ionomer on the Performance of Copper Catalyst Layers for CO₂ Electrolysis to Multicarbon Products

Idros, Mohamed Nazmi (author), Wu, Yuming (author), Duignan, Timothy (author), Li, Mengran (author), Cartmill, Hayden (author), Maglaya, Irving (author), Burdyny, T.E. (author), Wang, Geoff (author), Rufford, Thomas E. (author)

To explore the effects of solvent-ionomer interactions in catalyst inks on the structure and performance of Cu catalyst layers (CLs) for CO₂ electrolysis, we used a “like for like” rationale to select acetone and methanol as dispersion solvents with a distinct affinity for the ionomer backbone or sulfonated ionic heads,...

journal article 2023

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Effects of microporous layer on electrolyte flooding in gas diffusion electrodes and selectivity of CO₂ electrolysis to CO

Wu, Yuming (author), Garg, Sahil (author), Li, Mengran (author), Idros, Mohamed Nazmi (author), Li, Zhiheng (author), Lin, Rijia (author), Chen, Jian (author), Wang, Guoxiong (author), Rufford, Thomas E. (author)

Understanding the relationship between gas diffusion electrode (GDE) structures and the performance of electrochemical CO₂ reduction reaction (CO₂RR) is crucial to developing industrial-scale technologies to convert CO₂ to valuable products. We studied how the microporous layer (MPL) on GDE's coated with...

journal article 2022

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Electrochemical CO₂ reduction in membrane-electrode assemblies

Ge, Lei (author), Rabiee, Hesamoddin (author), Li, Mengran (author), Subramanian, S.S. (author), Zheng, Yao (author), Lee, Joong Hee (author), Burdyny, T.E. (author), Wang, H. (author)

Electrochemical conversion of gaseous CO₂ to value-added products and fuels is a promising approach to achieve net-zero CO₂ emission energy systems. Significant efforts have been achieved in the design and synthesis of highly active and selective electrocatalysts for this reaction and their reaction mechanism. To perform...

review 2022

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Regulating the reaction zone of electrochemical CO₂ reduction on gas-diffusion electrodes by distinctive hydrophilic-hydrophobic catalyst layers

Rabiee, Hesamoddin (author), Ge, Lei (author), Zhao, Jing (author), Zhang, Xueqin (author), Li, Mengran (author), Hu, Shihu (author), Smart, Simon (author), Rufford, Thomas E. (author), Zhu, Zhonghua (author)

Regulating the rational wettability on gas-diffusion electrodes (GDEs) plays a pivotal role to improve the efficiency of CO₂RR via fine-tuning the reaction zone and boosting the formation of triple-phase interfaces. Herein, we present a wettability regulation strategy that modulates the triple-phase reaction zone in the catalyst...

journal article 2022

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CO₂ Electrolysis via Surface-Engineering Electrografted Pyridines on Silver Catalysts

Abdinejad, M. (author), Irtem, I.E. (author), Farzi, Amirhossein (author), Sassenburg, M. (author), Subramanian, S.S. (author), Iglesias van Montfort, H.P. (author), Ripepi, D. (author), Li, Mengran (author), Middelkoop, J. (author), Seifitokaldani, Ali (author), Burdyny, T.E. (author)

The electrochemical reduction of carbon dioxide (CO₂) to value-added materials has received considerable attention. Both bulk transition-metal catalysts and molecular catalysts affixed to conductive noncatalytic solid supports represent a promising approach toward the electroreduction of CO₂. Here, we report a combined...

journal article 2022

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Mitigating Electrolyte Flooding for Electrochemical CO₂Reduction via Infiltration of Hydrophobic Particles in a Gas Diffusion Layer

Wu, Yuming (author), Charlesworth, Liam (author), Maglaya, Irving (author), Idros, Mohamed Nazmi (author), Li, Mengran (author), Burdyny, T.E. (author), Wang, Geoff (author), Rufford, Thomas E. (author)

Achieving operational stability at high current densities remains a challenge in CO2 electrolyzers due to flooding of the gas diffusion layer (GDL) that supports the electrocatalyst. We mitigated electrode flooding at high current densities using a vacuum-assisted infiltration method to embed 200-400 nm-sized polytetrafluoroethylene (PTFE)...

journal article 2022

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Energy comparison of sequential and integrated CO₂ capture and electrochemical conversion

Li, Mengran (author), Irtem, I.E. (author), Iglesias van Montfort, H.P. (author), Abdinejad, M. (author), Burdyny, T.E. (author)

Integrating carbon dioxide (CO2) electrolysis with CO2 capture provides exciting new opportunities for energy reductions by simultaneously removing the energy-demanding regeneration step in CO2 capture and avoiding critical issues faced by CO2 gas-fed electrolysers. However, understanding the potential energy advantages of an integrated...

journal article 2022

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Geometric Catalyst Utilization in Zero-Gap CO₂Electrolyzers

Subramanian, S.S. (author), Yang, K. (author), Li, Mengran (author), Sassenburg, M. (author), Abdinejad, M. (author), Irtem, I.E. (author), Middelkoop, J. (author), Burdyny, T.E. (author)

The electrochemical reduction of CO2 (CO2RR) on silver catalysts has been demonstrated under elevated current density, longer reaction times, and intermittent operation. Maintaining performance requires that CO2 can access the entire geometric catalyst area, thus maximizing catalyst utilization. Here we probe the time-dependent factors...

journal article 2022

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Advancing integrated CO₂ electrochemical conversion with amine-based CO₂ capture: a review

Li, Mengran (author), Yang, K. (author), Abdinejad, M. (author), Zhao, Chuan (author), Burdyny, T.E. (author)

Carbon dioxide (CO₂) electrolysis is a promising route to utilise captured CO₂ as a building block to produce valuable feedstocks and fuels such as carbon monoxide and ethylene. Very recently, CO₂ electrolysis has been proposed as an alternative process to replace the amine recovery unit of the commercially...

review 2022

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Urea-Functionalized Silver Catalyst toward Efficient and Robust CO₂ Electrolysis with Relieved Reliance on Alkali Cations

Garg, Sahil (author), Li, Mengran (author), Hussain, Tanveer (author), Idros, Mohamed Nazmi (author), Wu, Yuming (author), Zhao, Xiu Song (author), Wang, Geoff G.X. (author), Rufford, Thomas E. (author)

We report a new strategy to improve the reactivity and durability of a membrane electrode assembly (MEA)-type electrolyzer for CO2 electrolysis to CO by modifying the silver catalyst layer with urea. Our experimental and theoretical results show that mixing urea with the silver catalyst can promote electrochemical CO2 reduction (CO2R),...

journal article 2022

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In operando-formed interface between silver and perovskite oxide for efficient electroreduction of carbon dioxide to carbon monoxide

Wu, Xinhao (author), Guo, Y. (author), Gu, Yuxing (author), Xie, Fenghua (author), Li, Mengran (author), Hu, Zhiwei (author), Lin, Hong Ji (author), Pao, Chih Wen (author), Huang, Yu Cheng (author)

Electrochemical carbon dioxide (CO₂) reduction (ECR) is a promising technology to produce valuable fuels and feedstocks from CO₂. Despite large efforts to develop ECR catalysts, the investigation of the catalytic performance and electrochemical behavior of complex metal oxides, especially perovskite oxides, is rarely...

journal article 2022

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Cation-Driven Increases of CO₂Utilization in a Bipolar Membrane Electrode Assembly for CO₂Electrolysis

Yang, K. (author), Li, Mengran (author), Subramanian, S.S. (author), Blommaert, M.A. (author), Smith, W.A. (author), Burdyny, T.E. (author)

Advancing reaction rates for electrochemical CO2 reduction in membrane electrode assemblies (MEAs) have boosted the promise of the technology while exposing new shortcomings. Among these is the maximum utilization of CO2, which is capped at 50% (CO as targeted product) due to unwanted homogeneous reactions. Using bipolar membranes in an MEA ...

journal article 2021

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The role of electrode wettability in electrochemical reduction of carbon dioxide

Li, Mengran (author), Idros, Mohamed Nazmi (author), Wu, Yuming (author), Burdyny, T.E. (author), Garg, Sahil (author), Zhao, Xiu Song (author), Wang, Geoff (author), Rufford, Thomas E. (author)

The electrochemical reduction of carbon dioxide (CO₂RR) requires access to ample gaseous CO₂and liquid water to fuel reactions at high current densities for industrial-scale applications. Substantial improvement of the CO₂RR rate has largely arisen from positioning the catalyst close to gas-liquid interfaces,...

review 2021