Article
Electrochemistry
Rokas Zalneravicius, Arunas Ramanavicius
Summary: In this study, a Spirulina-based lysate was utilized as a redox mediator to design a glucose oxidase bioanode. The use of eco-friendly algae cell-based lysate facilitated electron transfer and enzyme immobilization, improving the performance of the bioanode. The designed bioanode exhibited high open circuit potential and power output, making it suitable for biofuel cell and glucose biosensor applications.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
John C. Ruth, Alfred M. Spormann
Summary: This article outlines the catalytic properties of electroactive enzymes in redox reactions and highlights their potential in environmentally friendly production of industrial chemicals. The authors discuss the current challenges in achieving high catalytic rates and stability, as well as two promising improvements in existing enzymatic electrochemical systems.
Article
Chemistry, Multidisciplinary
Christina Felbek, Steffen Hardt, Cecilia Papini, Debajyoti Pramanik, Vincent Artero, Marc Fontecave, Vincent Fourmond, Nicolas Plumere, Christophe Leger
Summary: Through experiments under conditions of mediated electron transfer, we have demonstrated that the dinuclear active site of [FeFe] hydrogenase can be inserted into the apo-enzyme embedded in a film of redox polymer, with maturation monitored by electrochemistry at a rate comparable to direct electron transfer. This new approach paves the way for the implementation of hydrogenases in large scale real-life processes.
CHEMICAL COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Steffen Hardt, Stefanie Stapf, Dawit T. Filmon, James A. Birrell, Olaf Ruediger, Vincent Fourmond, Christophe Leger, Nicolas Plumere
Summary: The research describes a redox-active film for bidirectional and reversible hydrogen conversion, which can be used for electrocatalytic energy conversion. By serving as both the anode material and a highly energy efficient cathode material in a biofuel cell, the film demonstrates high performance. The understanding of reversibility through a kinetic model has simplified the design principles of highly efficient and stable bioelectrocatalytic films.
Article
Chemistry, Multidisciplinary
Claudia Brocks, Chandan K. Das, Jifu Duan, Shanika Yadav, Ulf-Peter Apfel, Subhasri Ghosh, Eckhard Hofmann, Martin Winkler, Vera Engelbrecht, Lars V. Schaefer, Thomas Happe
Summary: This study proposes a new strategy to improve the O-2 stability of [FeFe]-hydrogenases by blocking the O-2 diffusion pathway and protecting the catalytic cofactor.
Article
Materials Science, Multidisciplinary
Yixuan Huang, Tsukuru Masuda, Madoka Takai
Summary: The modifiable polymer gel composed of phosphorylcholine and N-hydroxysuccinimide ester can be postmodified to obtain a redox zwitterionic gel, which demonstrates superior operational stability and resistance to biofouling compared to typical redox hydrogels. The gel can serve as an enzyme-immobilizing matrix for enzymatic bioelectrodes, showing potential applications in the field of implantable bioelectronic applications.
ACS APPLIED POLYMER MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Motaher M. Hossain, Jannatul Morshed, Seiya Tsujimura
Summary: A bio-conjugated redox network matrix has been developed on a glassy carbon electrode through covalent bonding with one-pot crosslinking, using glucose dehydrogenase, thionine, and poly(ethylene glycol) diglycidyl ether as components. This matrix allows for a glucose oxidation current of 400 mu A cm(-2) at 25 degrees C, with electrons from the enzyme diffusing through the network.
CHEMICAL COMMUNICATIONS
(2021)
Article
Biotechnology & Applied Microbiology
Jaehyun Cha, Jinhee Lee, Byoung Wook Jeon, Yong Hwan Kim, Inchan Kwon
Summary: This study proposes a CO2 hydrogenation system that utilizes hydrogenase from Ralstonia eutropha H16 (ReSH) and formate dehydrogenase from Methylobacterium extorquens AM1 (MeFDH1) to efficiently convert carbon dioxide in industrial flue gas into formate via a nicotinamide adenine dinucleotide-dependent cascade reaction. The enzyme system is tolerant to inhibitors such as carbon monoxide and oxygen, and it can utilize diverse sources of hydrogen and carbon dioxide.
FRONTIERS IN BIOENGINEERING AND BIOTECHNOLOGY
(2023)
Article
Biophysics
Zepeng Kang, Yuanming Wang, Haiyan Song, Xueli Wang, Job Zhang, Zhiguang Zhu
Summary: By designing a wearable and flexible lactic-acid/O2 EBFC with an air-breathing biocathode, the limitations of biocathode are effectively solved. The optimal performance conditions are determined through experiments, and the EBFC is successfully applied to power a low-power device.
BIOSENSORS & BIOELECTRONICS
(2024)
Article
Chemistry, Analytical
Roy Cohen, Rachel E. Bitton, Nidaa S. Herzallh, Yifat Cohen, Omer Yehezkeli
Summary: Flavin-dependent glucose dehydrogenases are explored for potential applications as biocatalysts in glucose biosensing. A thermophilic variant of the enzyme from Talaromyces emersonii was used in constructing an amperometric biosensor and a biofuel cell device, showing high bioelectrocatalytic activity and stability in various configurations. The biosensor also exhibited significant bioelectrocatalytic current responses in interstitial fluid-like solutions and generated power in the biofuel cell device.
ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Physical
Mathanraj Vijayaragavan, Balaji Subramanian, S. Sudhakar, L. Natrayan
Summary: This study investigates the performance, emission, and combustion characteristics of a compression ignition engine operating on dual fuel mode with simarouba oil, hydrogen, and exhaust gas recirculation (EGR). The results show that the introduction of hydrogen and EGR can improve the engine efficiency and reduce emissions.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Multidisciplinary
Ahmad Jaradat, Chengji Zhang, Sachin Kumar Singh, Junaid Ahmed, Alireza Ahmadiparidari, Leily Majidi, Sina Rastegar, Zahra Hemmat, Shuxi Wang, Anh T. Ngo, Larry A. Curtiss, Matthew Daly, Arunkumar Subramanian, Amin Salehi-khojin
Summary: A cost-effective, flexible, and wearable Li-O-2 battery has been designed in this study, which can operate in pure oxygen, dry air, and ambient air. The battery demonstrates excellent cycling and electrochemical performance, showing potential for applications in flexible and wearable electronics.
Article
Chemistry, Physical
Yuanming Wang, Yunhong Song, Chunling Ma, Zepeng Kang, Zhiguang Zhu
Summary: A thermophilic archaea host system was developed to express a thermostable Pyrococcus furiosus cytoplasmic [NiFe]-hydrogenase I, which showed high activity and stability at elevated temperatures. The recombinant hydrogenase could be a good candidate for catalyzing H-2/air biofuel cells, with promising electrochemical performance and oxygen tolerance.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Multidisciplinary
Jin Zhang, Yuping Cao, Wei Liu, Ting Cao, Jing Qian, Jiemin Wang, Xiaojun Yao, Anam Iqbal, Wenwu Qin
Summary: The simultaneous presence of triazine and ketone acceptors in covalent organic frameworks has been found to enhance electron-hole separation efficiency and improve photocatalytic hydrogen production. COFs with two acceptors showed the highest hydrogen production rate. A single phenyl group as a bridging unit was more favorable for the catalytic reaction, indicating the importance of distance between acceptors in COF design.
Article
Chemistry, Physical
Mira T. Gamache, Rima Charaf, Larissa Kurth, Dawit T. Filmon, Moritz Senger, Nicolas Plumere, Leif Hammarstrom, Gustav Berggren
Summary: In this study, a semi-artificial photocatalytic system using Escherichia coli bacteria as the catalyst for hydrogen gas production was investigated. The addition of a redox mediator greatly improved the efficiency of the system, but also negatively affected the integrity and viability of E. coli cells. Spectroscopic analysis was used to study the influence of photochemistry on the system performance.
Article
Biophysics
Kavita Jayakumar, Anna Lielpetere, Daniel A. Domingo-Lopez, Ruth E. Levey, Garry P. Duffy, Wolfgang Schuhmann, Donal Leech
Summary: Foreign body response (FBR) is a challenge for implantable biosensors and medical devices. Zwitterionic polymers (ZPs) show promise in reducing biofouling. A ZP containing MPC was found to effectively resist fibrinogen adsorption and fibroblast adhesion, while maintaining sensor performance.
BIOSENSORS & BIOELECTRONICS
(2023)
Article
Chemistry, Multidisciplinary
Swapnil Varhade, E. B. Tetteh, Sascha Saddeler, Simon Schumacher, H. B. Aiyappa, Georg Bendt, Stephan Schulz, Corina Andronescu, Wolfgang Schuhmann
Summary: Scanning electron microscopy and atomic force microscopy images of droplet landing sites are correlated with the electrocatalytic activity for the oxygen evolution reaction in alkaline electrolyte of hexagonal spinel Co3O4 nanoparticles derived using scanning electrochemical cell microscopy. The turnover frequency (TOF) of surface Co atoms is used to deconvolute the intrinsic catalytic activity of individual crystal facets of the hexagonal Co3O4 spinel particle. The top surface exposing 111 crystal planes showed a thickness-dependent TOF, while the edge of the particle exposing (110) planes showed a higher average TOF and no correlation with particle thickness.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Xin Wang, Wenhui He, Jialin Shi, Joao R. C. Junqueira, Jian Zhang, Stefan Dieckhoefer, Sabine Seisel, Debanjan Das, Wolfgang Schuhmann
Summary: In this study, an Ag-Bi2O3 hybrid nanofiber was developed for highly efficient electrochemical reduction of CO2 to formate. The Ag-Bi2O3 catalyst exhibited a formate selectivity of over 90%, and achieved a yield rate of 11.7 mmol·s(-1)·m(-2) at a current density of -250 mA·cm(-2). The presence of Ag in the catalyst increased the energy efficiency by nearly 10% compared to a Bi2O3 only counterpart, and this enhancement was attributed to the conversion of Bi2O3 from a monoclinic phase to a metastable tetragonal phase and the accelerated formation of active metallic Bi at low overpotentials.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Physical
Samuel V. Somerville, Peter B. O'Mara, Tania M. Benedetti, Soshan Cheong, Wolfgang Schuhmann, Richard D. Tilley, J. Justin Gooding
Summary: Enzymes with multiple active sites and control over the solution environment enable the formation of complex products from simple reactants. We mimic this concept using nanoparticles to facilitate the electro-chemical carbon dioxide reduction reaction. By altering the rate of CO2 delivery, the activity of the CO producing site, and the applied potential, we show that stable nanoparticles with lower CO formation activity can produce greater amounts of hydrocarbon products. This highlights the importance of the local solution environment and the stability of the catalyst in cascade reactions.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Wenhui He, Shubhadeep Chandra, Thomas Quast, Swapnil Varhade, Stefan Dieckhoefer, Joao R. C. Junqueira, Huimin Gao, Sabine Seisel, Wolfgang Schuhmann
Summary: Renewable electricity-powered nitrate reduction reaction (NO3RR) offers a net-zero carbon route to high ammonia (NH3) productivity. However, this route suffers from low energy efficiency due to the need for high overpotentials. A rational catalyst design strategy involving the assembly of Cu/Co nanophases into nanoribbons is suggested to alleviate this issue. Experimental studies show that the Cu-Co nanoribbons enable strong NO3- adsorption and rapid catalysis of NO3- to NH3, achieving a stable NO3RR with high current density and Faradaic efficiency.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Chenglong Luan, Johanna Angona, Arjun Bala Krishnan, Manuel Corva, Pouya Hosseini, Markus Heidelmann, Ulrich Hagemann, Emmanuel Batsa Tetteh, Wolfgang Schuhmann, Kristina Tschulik, Tong Li
Summary: We investigated the relationship between crystallographic orientations of beta-CoOOH and catalytic activity for the oxygen evolution reaction (OER). We found that beta-CoOOH(01 1? ${\bar{1}}$ 0) grown on [ 1?21? ${\bar{1}2\bar{1}}$ 0]-oriented Co exhibited higher OER activity compared to beta-CoOOH(10 1? ${\bar{1}}$ 3) grown on [02 2?1] ${\bar{2}1]}$ -oriented Co or beta-CoOOH(0006) grown on [0001]-oriented Co. This is due to the presence of higher amounts of hydroxyl ions and more easily reducible Co-III-O sites in beta-CoOOH(01 1? ${\bar{1}}$ 0). Our findings offer opportunities for designing pre-catalysts with preferred defects to promote the formation of the most active OER species.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Carla Santana Santos, Bright Nsolebna Jaato, Ignacio Sanjuan, Wolfgang Schuhmann, Corina Andronescu
Summary: Scanning electrochemical probe microscopy (SEPM) techniques are used to study the local electrochemical reactivity of interfaces. Operando SEPM measurements involve using a SEPM tip to investigate electrocatalysts' performance while modulating the interface reactivity. This combination allows the correlation of electrochemical activity with changes in surface properties and provides insights into reaction mechanisms.
Article
Chemistry, Physical
Panpan Wang, Anna Frank, Jens Appel, Marko Boehm, Nadine Strabel, Marc M. Nowaczyk, Wolfgang Schuhmann, Felipe Conzuelo, Kirstin Gutekunst
Summary: Photosynthetic hydrogen production is achieved by coupling the hydrogenase enzyme to photosystem I, which allows for efficient storage of solar energy. In this study, a system combining in vivo and in vitro approaches is established to produce photoH(2). The in vivo assembly ensures functionality of the chimeric protein, while the in vitro characterization allows for detailed analysis. This approach opens avenues for optimizing photoH(2) production in the future.
ADVANCED ENERGY MATERIALS
(2023)
Article
Electrochemistry
Ndrina Limani, Emmanuel Batsa Tetteh, Moonjoo Kim, Thomas Quast, Emmanuel Scorsone, Bruno Jousselme, Wolfgang Schuhmann, Renaud Cornut
Summary: Carbon-based nanomaterials are excellent candidates for oxygen reduction reaction (ORR) electrocatalysis due to their exceptional properties. However, investigating their intrinsic activity can be challenging using conventional methodologies. This study employs nano-scale scanning electrochemical cell microscopy (SECCM) to investigate individual catalyst agglomerates, providing high-resolution electrochemical information. The intrinsic ORR activity of the catalyst is revealed by normalizing the data based on their distinctive electrochemical surface area (ECSA). Additionally, the structure and morphology of the catalytically active agglomerates are visualized using scanning electron microscopy (SEM).
Article
Chemistry, Multidisciplinary
Anna Lielpetere, Kavita Jayakumar, Donal Leech, Wolfgang Schuhmann
Summary: Polymer coatings can protect redox polymer-based glucose biosensors from interference and prolong their functional lifetime. Different approaches were explored to protect against different interferents, and a multi-layer polymer design showed the best protection against AA, UA, and biological interferences.
Article
Chemistry, Multidisciplinary
Muhammad Adib Abdillah Mahbub, Joao R. C. Junqueira, Xin Wang, Jian Zhang, Stefan Dieckhoefer, Sabine Seisel, Debanjan Das, Wolfgang Schuhmann
Summary: A facile strategy of using 2-methyl-imidazole coordinated to Bi to boost CO2 reduction to formate with high selectivity and activity is reported.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Moonjoo Kim, Emmanuel Batsa Tetteh, Olga A. Krysiak, Alan Savan, Bin Xiao, Tobias Horst Piotrowiak, Corina Andronescu, Alfred Ludwig, Taek Dong Chung, Wolfgang Schuhmann
Summary: Using scanning electrochemical cell microscopy (SECCM), the PZC and HER activities of various elemental compositions of a Pt-Pd-Ru-Ir-Ag thin-film HEA materials library (HEA-ML) were determined. The PZC of Pt-Pd-Ru-Ir-Ag is linearly correlated with its composition-weighted average work function. The HER current density in acidic media positively correlates with the PZC, which can be explained by the preconcentration of H+ in the electrical double layer at potentials negative of the PZC.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Christian M. Clausen, Olga A. Krysiak, Lars Banko, Jack K. Pedersen, Wolfgang Schuhmann, Alfred Ludwig, Jan Rossmeisl
Summary: Compositionally complex materials, such as high-entropy alloys and oxides, have the potential to be efficient catalyst platforms due to their vast chemical space. However, determining the composition of active catalyst materials requires understanding the descriptor-activity relationship, which is challenging experimentally. In this study, we show that inferred adsorption energy distributions on complex solid solution surfaces can predict the electrocatalytic performance of oxygen reduction reaction in the Ag-Pd-Pt-Ru system with high accuracy.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Alexander Gunnarson, Thomas Quast, Stefan Dieckhoefer, Norbert Pfaender, Ferdi Schueth, Wolfgang Schuhmann
Summary: This study investigates the stability of catalysts in Proton Exchange Membrane Fuel Cells (PEMFCs). The research finds that the degradation of catalysts is accelerated due to locally different pH values. It also raises concerns about the applicability of accelerated stress tests for evaluating catalyst stability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Electrochemistry
Swapnil Varhade, Gabriel Meloni, Emmanuel Batsa Tetteh, Monjoo Kim, Simon Schumacher, Thomas Quast, Corina Andronescu, Patrick Unwin, Wolfgang Schuhmann
Summary: Scanning electrochemical cell microscopy (SECCM) was used to investigate the interaction between aqueous alkaline electrolyte and a glassy carbon electrode surface. Numerical simulations were performed to study the impact of droplet geometry and size on the voltammetric signature. The study provides insights into droplet-surface interactions, which are crucial for a quantitative interpretation of SECCM measurements.
ELECTROCHIMICA ACTA
(2023)
