Article
Chemistry, Multidisciplinary
Hugh Warkentin, Colin P. O'Brien, Sarah Holowka, Benjamin Maxwell, Mariam Awara, Mark Bouman, Ali Shayesteh Zeraati, Rachael Nicholas, Alexander H. Ip, Essam S. Elsahwi, Christine M. Gabardo, David Sinton
Summary: The stability of CO2RR electrolyzers remains a challenge. This study demonstrates the continuous monitoring of electrolyzers using real-time electrochemical impedance spectroscopy (EIS) analysis, identifying common failure modes and proposing a framework for predicting and preventing failures.
Article
Chemistry, Multidisciplinary
Chanjuan Zhang, Philipp Gotico, Regis Guillot, Diana Dragoe, Winfried Leibl, Zakaria Halime, Ally Aukauloo
Summary: At the core of carbon monoxide dehydrogenase (CODH) active site, two metal ions and hydrogen bonding from amino acids facilitate the interconversion between CO2 and CO. A designed molecular catalyst with a bimetallic iron complex and hydrogen bonding interactions showed improved selectivity and stability in heterogeneous CO2 reduction to CO. X-ray structures revealed the compromise between rigidity and flexibility of the catalyst in accommodating CO2 capture, activation, and reduction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Xiaolong Zhang, Chuangwei Liu, Yong Zhao, Linbo Li, Yu Chen, Fazal Raziq, Liang Qiao, Si-Xuan Guo, Caiyun Wang, Gordon G. Wallace, Alan M. Bond, Jie Zhang
Summary: This work introduces a coordination enabled galvanic replacement method to decorate atomic Ni clusters on defect-rich Cu surface, resulting in significant enhancement of C2 products production in electrocatalytic CO2 reduction. With a surface Ni/Cu ratio of 0.82 %, a 7-fold increase in selectivity for C2 products was observed compared to pristine Cu, attributed to the chemisorption of CO2 on Ni decorated surfaces changing the rate determining step for *CO formation. The catalytic mechanism demonstrated in the Cu-Ni system points to new directions for the development of advanced bimetallic electrocatalysts for producing multi-carbon materials from CO2 reduction.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Inorganic & Nuclear
Zhixiang Zhou, Fengshou Yu, Yang You, Jiayu Zhan, Lu-Hua Zhang
Summary: By anchoring CoPc complex on an MXene support with different terminal groups (-F or -OH), the effect of the terminal groups on the performance of the electrochemical CO2 reduction reaction (ECRR) was systematically studied. The results showed that CoPc/MXene-OH exhibited a higher faradaic efficiency for CO formation (FECO) of 92.4% compared to CoPc/MXene-F (84.0%) under the same conditions. Mechanistic exploration indicated that the excellent performance was attributed to the electron-donating property of -OH, which enriched the electron density of Co and optimized the binding strength for intermediates.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Yize Zhang, Hangshuai Li, Xingyue He, Aiqing Wang, Guoyi Bai, Xingwang Lan
Summary: This study reports the synthesis of a crystalline 2,2'-bipyridine-based covalent organic framework bearing Cd single-atom sites (Cd-Bpy-COF) as a synergistic catalyst for carboxylative cyclization with CO2. The integration of COF framework and single Cd active sites remarkably boosts the adsorption and activation of CO2, promoting its following cyclization reaction. This study further demonstrates the designed possibility of COF catalysts for high-performance CO2 conversion.
Article
Engineering, Environmental
Yan Resing Dias, Oscar W. Perez-Lopez
Summary: Mitigating CO2 emissions has become an important issue nowadays, and converting CO2 to CH4 as a natural gas substitute and H2 storage source is an interesting alternative. In this study, Ni/SiO2 catalysts promoted by Fe, Co and Zn were prepared and showed improved performance in CO2 conversion to methane, with Ni-Co/SiO2 achieving the best results in terms of CO2 conversion and CH4 selectivity.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Chemistry, Analytical
Yang Yue, Xiaohuan Zou, Yuande Shi, Jiannan Cai, Yuxuan Xiang, Zhongshui Li, Shen Lin
Summary: In this study, a low crystallinity CuO-SnO2/C catalyst was synthesized by integrating CuO and SnO2 on carbon black, which exhibited significantly enhanced selectivity, activity, and stability towards the reduction of carbon dioxide. The well-distributed CuO and SnO2 nanoparticles on carbon black resulted in a larger electrochemically active surface area (ECSA) and faster electron transfer capacity, contributing to the enhanced electrocatalytic process. The low crystallinity of CuO on CuO-SnO2/C facilitated the easier electron transfer to the CO2 surface, accelerating the reduction reaction. The obtained CuO-SnO2/C with low crystallinity efficiently catalyzed the reduction of CO2 to formic acid and syngas, with a high Faradaic efficiency (FE) of C1 products (HCOOH + CO) of 80%, and 100% FE can be utilized.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Physical
Hyunsu Han, Juhwan Im, Myungsuk Lee, Daehyun Choo
Summary: In this study, highly efficient diatomic electrocatalysts with Ni and Mn single-atom pair sites were synthesized on N-doped porous carbon framework for CO2 conversion. The resulting catalysts exhibited a high Faradaic efficiency and industrially relevant current density. The experimental measurements and theoretical calculations revealed that the synergistic electronic modification effect of neighboring Ni and Mn single atoms played a favorable role in the reaction steps of CO2 conversion.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Review
Chemistry, Physical
Zhiyong Qiao, Changming Ding
Summary: This article provides a systematic review of carbon fibers and their applications in electrocatalytic reactions. It discusses the synthesis strategy, properties, and crucial role of carbon fibers in driving electrocatalytic reactions, and explores the challenges and prospects of fiber materials in electrocatalysis applications.
Article
Chemistry, Multidisciplinary
Tewodros Asefa, Chaoyun Tang, Maricely Ramirez-Hernandez
Summary: The growing energy demand worldwide has led to increased use of fossil fuels, which is depleting faster and causing more negative environmental impacts. Alternative, environmentally friendly energy sources such as fuel cells and electrolyzers are being developed. Significant progress has been made in this area, though challenges remain in scaling up such energy systems due to their noble metal catalysts.
Article
Chemistry, Physical
Juqin Zeng, Marco Fontana, Micaela Castellino, Adriano Sacco, M. Amin Farkhondehfal, Filippo Drago, Candido Fabrizio Pirri
Summary: This study demonstrates that bimetallic copper-tin catalysts with specific Cu to Sn ratios can effectively enhance the CO2 reduction reaction with excellent CO selectivity and high stability. The catalyst is characterized by its simple synthesis process, low cost, superior performance, making it suitable for large-scale CO2 electrolyzers.
Review
Green & Sustainable Science & Technology
Shanwen Wang, Tianyi Kou, Sarah E. Baker, Eric B. Duoss, Yat Li
Summary: This article introduces the advantages of electrochemical CO2 reduction in generating value-added products and mitigating climate change, with a focus on CO2RR catalysts that exhibit high selectivity and activity in alcohol production. The current understanding of reaction pathways on different catalyst surfaces and strategies to enhance CO2RR catalytic performance are discussed. Finally, the challenges and possible future paths for the field are shared.
ADVANCED ENERGY AND SUSTAINABILITY RESEARCH
(2022)
Review
Chemistry, Physical
Fu Liu, Jingwen Zhou, Yunhao Wang, Yuecheng Xiong, Fengkun Hao, Yangbo Ma, Pengyi Lu, Juan Wang, Jinwen Yin, Guozhi Wang, Jinli Yu, Yan Yan, Zonglong Zhu, Jie Zeng, Zhanxi Fan
Summary: Metal-CO2 batteries (MCBs) are expected to address environmental and energy crises by integrating CO2 conversion and renewable energy storage. Catalyst cathodes based on 2D materials offer great opportunities in designing high-performance MCBs, showing superior electrocatalytic capacity. This review presents the cutting-edge progresses of 2D materials-based catalyst cathodes in MCBs, including reaction mechanisms, design criteria, and engineering strategies for high-performance MCBs.
Article
Chemistry, Physical
Hyunsu Han, Song Jin, Seongmin Park, Yoongon Kim, Daehee Jang, Min Ho Seo, Won Bae Kim
Summary: Oxygen vacancy engineering is a new direction for designing high-performance catalysts for electrochemical CO2 reduction. Amorphous MnOx catalysts with different concentrations of oxygen vacancies were prepared, with the high vacancy catalyst showing superior CO2 to CO conversion efficiency. This enhancement is attributed to the oxygen vacancies facilitating CO2 adsorption/activation and promoting charge transfer for efficient CO2 reduction.
Article
Electrochemistry
Ana Marija Damjanovic, Burak Koyutuek, Yan-Sheng Li, Davide Menga, Christian Eickes, Hany A. El-Sayed, Hubert A. Gasteiger, Tim-Patrick Fellinger, Michele Piana
Summary: This study investigated the impact of catalyst loading on the mass activity of PGM-free ORR catalysts, revealing an independence of the ORR mass activity from the catalysts loading when corrections for voltage losses in H-2/O-2 single cell tests are considered. Additionally, no clear relation of stability to the catalyst loading was found in H-2/O-2 PEMFCs.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Taylor Uekert, Mark A. Bajada, Teresa Schubert, Christian M. Pichler, Erwin Reisner
Summary: Solar-driven reforming technology utilizes a photocatalyst to generate H-2 fuel from waste, facing challenges such as photocatalyst dispersion, light absorption competition, slow reaction rates, and low conversion yields. The immobilization of CNx|Ni2P photocatalyst on textured glass is shown to overcome these limitations, achieving efficient waste conversion.
Article
Chemistry, Physical
Philip M. Stanley, Christopher Thomas, Erling Thyrhaug, Alexander Urstoeger, Michael Schuster, Juergen Hauer, Bernhard Rieger, Julien Warnan, Roland A. Fischer
Summary: This study presents a novel approach to enhance photocatalytic CO2 reduction activity by embedding a molecular catalyst in a metal-organic framework. The ratio of immobilized catalyst to photosensitizer is crucial for improving reaction efficiency and determining optimal performance, while the research also reveals the impact of reaction environment on active sites and provides a future direction for increasing turnover numbers.
Article
Chemistry, Physical
Vivek M. Badiani, Samuel J. Cobb, Andreas Wagner, Ana Rita Oliveira, Sonia Zacarias, Ines A. C. Pereira, Erwin Reisner
Summary: This study elucidates the key factors governing the activity and stability of immobilized redox enzymes and the role of film loss, particularly hydrogen bonding, in stabilizing bioelectrode performance. Electrostatic interactions are responsible for enzyme orientation, while hydrogen bonding limits enzyme desorption and improves enzyme stability.
Article
Chemistry, Multidisciplinary
Shujin Hou, Lili Xu, Xing Ding, Regina M. Kluge, Theophilus Kobina Sarpey, Richard W. Haid, Batyr Garlyyev, Soumya Mukherjee, Julien Warnan, Max Koch, Shengli Zhang, Weijin Li, Aliaksandr S. Bandarenka, Roland A. Fischer
Summary: Understanding the electrode/electrolyte interface is crucial for optimizing electrocatalytic performances. The nature of alkali metal cations has been found to have a profound impact on the oxygen evolution activity of SURMOF derived electrocatalysts based on NiFe(OOH). The effects of cation-dependent electric double layer properties on activity were studied using a laser-induced current transient technique. Electrolyte composition can be used to maximize the performance of SURMOF derivatives in electrochemical water splitting.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Samuel J. Cobb, Vivek M. Badiani, Azim M. Dharani, Andreas Wagner, Sonia Zacarias, Ana Rita Oliveira, Ines A. C. Pereira, Erwin Reisner
Summary: The effect of CO2 hydration on enzymatic and heterogeneous CO2 reduction has been studied. Co-immobilization of carbonic anhydrase can increase CO2 hydration kinetics, benefiting enzymatic catalysis but detrimental to heterogeneous catalysis.
Article
Multidisciplinary Sciences
Virgil Andrei, Geani M. Ucoski, Chanon Pornrungroj, Chawit Uswachoke, Qian Wang, Demetra S. Achilleos, Hatice Kasap, Katarzyna P. Sokol, Robert A. Jagt, Haijiao Lu, Takashi Lawson, Andreas Wagner, Sebastian D. Pike, Dominic S. Wright, Robert L. Z. Hoye, Judith L. MacManus-Driscoll, Hannah J. Joyce, Richard H. Friend, Erwin Reisner
Summary: Photocathodes deposited on thin and flexible substrates achieved high activity for hydrogen production and high selectivity for CO2 reduction. The corresponding lightweight perovskite-BiVO4 PEC devices demonstrated promising solar-to-fuel efficiencies and potential for scalability. The use of lightweight reactors and the ability to float in water make them suitable for open-water applications.
Article
Chemistry, Multidisciplinary
Philip M. Stanley, Florian Sixt, Julien Warnan
Summary: This study demonstrates the specific confinement of a rhenium coordination complex in a metal-organic framework (MOF) that enables unique electron accumulating property under visible-light irradiation. The material can concentrate and store electric charges for over four weeks without loss. It also allows decoupled, on-demand discharge for electrochemical reactions and H-2 evolution catalysis. Experimental investigations and theoretical calculations reveal the key role of MOF confinement on molecular guests in electron trapping.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Philip M. M. Stanley, Alice Y. Y. Su, Vanessa Ramm, Pascal Fink, Ceren Kimna, Oliver Lieleg, Martin Elsner, Johannes A. A. Lercher, Bernhard Rieger, Julien Warnan, Roland A. A. Fischer
Summary: A light-harvesting metal-organic framework has been engineered as a catalyst carrier, achieving controllable photocatalytic synthesis of syngas. This study is a significant breakthrough for photocatalytic CO2 reduction and H2 evolution in sustainable energy cycles.
ADVANCED MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
P. M. Stanley, J. Haimerl, N. B. Shustova, R. A. Fischer, J. Warnan
Summary: Solar fuel production through artificial molecular photosystems is attractive due to its potential to generate sustainable clean energy. The interface between molecular constituents and metal-organic frameworks (MOFs) allows for recyclability, controlled site positioning, and insights into catalytic mechanisms.
Review
Chemistry, Multidisciplinary
Vitthal B. Saptal, Vincenzo Ruta, Mark A. Bajada, Gianvito Vile
Summary: Single-atom catalysts have great potential in the chemical sector, pushing the boundaries of catalysis in new directions. These materials, consisting of isolated metal species ligated on solid supports, have various coordination environments and show important functions in specific transformations. This Review highlights the impressive progress made in using single-atom catalysts in organic synthesis and identifies potential knowledge gaps in the search for sustainable and earth-abundant catalysts for synthetic applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Xiaoxin Ma, Daniel J. J. Zheng, Shujin Hou, Soumya Mukherjee, Rachit Khare, Guanhui Gao, Qing Ai, Batyr Garlyyev, Weijin Li, Max Koch, Janos Mink, Yang Shao-Horn, Julien Warnan, Aliaksandr S. Bandarenka, Roland A. Fischer
Summary: Metal-organic frameworks (MOFs) have been used for catalyzing the oxygen evolution reaction (OER), but the critical factors determining OER performance are still not well understood. In this study, an isoreticular series of Ni-carboxylate-type MOFs was chosen to investigate the effects of carboxylate linker length and linker-linker pi-pi interactions on MOF degradation and reconstruction. The results showed that the linker controlled the transformation of MOF into different nickel hydroxide phases, which correlated the composition of Ni-MOF with the OER activity of the derived metastable nickel hydroxide phases.
Article
Chemistry, Multidisciplinary
Alessandra Sivo, Vincenzo Ruta, Vittoria Granata, Oleksandr Savateev, Mark A. Bajada, Gianvito Vile
Summary: Efficient catalytic methods for trifluoromethylation of (hetero)arenes play a crucial role in the production of organic and pharmaceutical compounds. Current protocols often rely on toxic reagents and expensive or difficult-to-handle catalysts. Carbon nitride, a non-toxic photocatalyst prepared from inexpensive precursors, offers a promising alternative. However, the relationship between physicochemical properties of carbon nitride and its catalytic performance remains poorly understood.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Ladawan Pukdeejorhor, Suttipong Wannapaiboon, Jan Berger, Katia Rodewald, Sutarat Thongratkaew, Sarawoot Impeng, Julien Warnan, Sareeya Bureekaew, Roland A. Fischer
Summary: Pre-designing starting materials is an effective strategy to enhance the activity of a photocatalyst without the need for additional active species. In this study, pre-designed titanium-oxo-carboxylate clusters were used to synthesize a metal-organic framework (MOF) photocatalyst MIL-125-(Ti)-NH2 for H-2 evolution. The resulting MOFs possessed abundant defects at the Ti centers, which acted as accessible active sites for H-2 generation. The use of pre-designed clusters also altered the electronic optical properties and energy levels, leading to a significantly higher H-2 evolution rate compared to the traditional hydrothermal synthesis method.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Philip M. Stanley, Karina Hemmer, Markus Hegelmann, Annika Schulz, Mihyun Park, Martin Elsner, Mirza Cokoja, Julien Warnan
Summary: The optimized catalyst materials for visible light-driven fuel production in porous host-guest systems have been studied, revealing the significant impact of MOF topology on the selectivity of solar fuel production.
Review
Chemistry, Multidisciplinary
Mark A. Bajada, Jesus Sanjose-Orduna, Giovanni Di Liberto, Sergio Tosoni, Gianfranco Pacchioni, Timothy Noel, Gianvito Vile
Summary: The global warming crisis has led to environmentally cautious trends in chemistry, prompting a rethinking of synthesis methods and catalyst design. Single-atom catalysis has merged the benefits of homogeneous and heterogeneous catalysis, but its current applications are limited to the energy sector. Further sustainable development is needed.
CHEMICAL SOCIETY REVIEWS
(2022)
