Article
Chemistry, Physical
Shi He, Yufeng Chen, Mengdi Wang, Hanggai Nuomin, Peter Novello, Xueqian Li, Siyuan Zhu, Jie Liu
Summary: Ammonia is a promising hydrogen mediator that reduces the cost of hydrogen transportation, but improvements are needed for extracting hydrogen. Ammonia electrolysis is a convenient method for low-cost hydrogen production. Nickel-cobalt nitride nanosheets show high electrocatalytic activity for the ammonia oxidation reaction in non-aqueous solutions.
Review
Chemistry, Multidisciplinary
Sebastian B. Beil, Dennis Pollok, Siegfried R. Waldvogel
Summary: The use of electric current as a traceless activator and reagent is experiencing a resurgence in the field of organic chemistry. With researchers from diverse scientific backgrounds entering this field, there is a diversity in reported parameters and methods, potentially impacting the reproducibility of electroorganic syntheses. This Review provides guidelines to streamline experimental parameters and improve reproducibility in the field.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Engineering, Environmental
Felix Holtkamp, Joachim Clemens, Manfred Trimborn
Summary: This study investigated the use of calcium cyanamide as a slurry additive to reduce ammonia and greenhouse gas emissions in agriculture, showing promising results.
Article
Green & Sustainable Science & Technology
Gruffydd Jones, John Scullion, Sarah Dalesman, Paul Robson, Dylan Gwynn-Jones
Summary: This study explores the potential of acidifying cattle slurry to enable the growth of Lemna minor on less diluted wastewater, which is typically toxic to the plant. By lowering the pH, the toxic NH3 form can be shifted towards the less toxic NH4+ form, allowing the plant to grow. This finding has important implications for implementing duckweed-based wastewater treatment systems in agriculture.
JOURNAL OF CLEANER PRODUCTION
(2023)
Review
Chemistry, Multidisciplinary
Marcella Bini, Marco Ambrosetti, Daniele Spada
Summary: Ferrites are ceramic oxides with intriguing physico-chemical properties that have been widely used in various applications. ZnFe2O4 and its solid solutions have drawn attention as anode materials for lithium-ion batteries due to their low cost, abundance, and high theoretical specific capacity.
APPLIED SCIENCES-BASEL
(2021)
Review
Chemistry, Multidisciplinary
Kai Chen, Dong-Yue Yang, Gang Huang, Xin-Bo Zhang
Summary: The development of high energy-density, low-cost, and safe batteries is crucial for technological innovation and changing human lifestyle. Lithium-air batteries are promising candidates for next-generation batteries due to their high energy density. However, research on lithium-air batteries is still in its early stages, with challenges including electrolyte decomposition and anode corrosion.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Review
Chemistry, Multidisciplinary
Emily R. Cooper, Ming Li, Ian Gentle, Qingbing Xia, Ruth Knibbe
Summary: Lithium and sodium metal batteries, as well as anode-free metal batteries, are important in battery research due to their high energy density. However, the uneven metal nucleation and growth hinder their commercialization. This review connects models and theories from metallurgy and electrodeposition to explain the driving forces behind uneven metal growth and provide guidance for future experiment design.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Applied
Artur Braun, Debajeet K. Bora, Lars Lauterbach, Elisabeth Lettau, Hongxin Wang, Stephen P. Cramer, Feipeng Yang, Jinghua Guo
Summary: This article discusses the importance of the 100th anniversary of CASALE SA, a leading nitrogen fixation technology developer, and solutions for sustainable ammonia production. The article reviews the role of nitrogen in photosynthesis and biology, as well as the use of ammonia as fertilizer and an energy carrier. It also introduces novel analytical techniques and provides real-world examples of ammonia production and usage.
Article
Chemistry, Physical
Riyi Chen, Songsheng Zheng, Yudong Yao, Zhibin Lin, Wei Ouyang, Lianghui Zhuo, Zhaolin Wang
Summary: Through investigating the performance of a direct ammonia fuel cell, it was found that the PtIr/C alloy catalyst achieved the highest peak power density and open-circuit voltage, but also showed a correlation between ammonia permeation and cathode catalyst degradation.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Review
Chemistry, Physical
Yiyin Huan, Aya Gomaa Abdelkader Mohamed, Jiafang Xie, Yaobing Wang
Summary: To develop and improve electrocatalysts for energy conversion, it is crucial to understand the active sites and their surface evolution under real operating conditions. Strategies to control the formation or reservation of stable highly-active sites include atomic/defective modulation, interfacial coupling, structural optimization, and forming a protective layer. Challenges remain in developing electrocatalysts with a clear structure-performance relationship and identifying real active sites after surface evolution.
Article
Physics, Applied
Kirk H. Bevan, Yee Wei Foong, Javad Shirani, Shuaishuai Yuan, Sinan Abi Farraj
Summary: This work explores the understanding of electrochemical tunneling reactions within the single-particle picture, based on the Gerischer-Hopfield description of electron transfer at solid-liquid interfaces. It discusses both single and multiple electron tunneling reactions, as well as related voltammetric concepts and trends. The impact of nuclear quantization on the Gerischer-Hopfield description and its representation of two probe electrochemical phenomena at low temperatures is addressed.
JOURNAL OF APPLIED PHYSICS
(2021)
Article
Chemistry, Inorganic & Nuclear
Zhaopeng Sun, Luojia Liu, Meng Zhang, Weiwei Huang
Summary: In this study, a new research approach was proposed to investigate the sodium storage mechanisms of small-molecule organic materials with complex structures. The redox-active sites for the sodiation process were predicted and the reasonable sequences of discharge sites were verified. The theoretical reduction potentials calculated showed high consistency with experimental data, providing insights for the theoretical investigation of the reduction mechanism and redox potential of small-molecule organic materials.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Review
Chemistry, Multidisciplinary
Yaowen Liu, Pengfei Li, Yanwei Wang, Youai Qiu
Summary: Electrochemistry employs electrons as an efficient and sustainable alternative to chemical oxidants or reductants, and has gained popularity for selective organic synthesis. The combination of electrochemistry with readily available electrophiles has emerged as a viable method for constructing challenging C-C and C-heteroatom bonds. This mini-review provides a systematic summary of the recent advances in electroreductive cross-electrophile coupling (eXEC) reactions, focusing on aryl and alkyl organic (pseudo)halides, as well as small molecules such as CO2, SO2, and D2O.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Physical
Peng Li, Hun Kim, Seung-Taek Myung, Yang-Kook Sun
Summary: This review highlights the necessity of co-exploitation of silicon and graphite, and systematically concludes the key issues, challenges, and perspectives of Si-graphite electrodes. Through a deep understanding of associated electrochemical processes, the component and structural optimization of Si-graphite anodes could be effectively enhanced.
ENERGY STORAGE MATERIALS
(2021)
Review
Chemistry, Physical
Ziga Ponikvar, Blaz Likozar, Saso Gyergek
Summary: The conventional method for synthesizing ammonia is costly and energy-intensive. Recent developments focus on alternative methods and electrification of ammonia production and decomposition.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Qiucheng Xu, Aoni Xu, Sahil Garg, Asger B. Moss, Ib Chorkendorff, Thomas Bligaard, Brian Seger
Summary: In this study, a descriptor called surface-accessible CO2 concentration ([CO2](SA)) was developed to indicate the limits of CO2-to-CO conversion in CO2 electrolysis. Three general strategies were identified to enrich [CO2](SA), resulting in improved performance. The maximum j(CO) achieved was 368 +/- 28 mA cm(geo)(-2) using a commercial silver catalyst.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Editorial Material
Chemistry, Physical
Jakob Kibsgaard, Ib Chorkendorff
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Asger B. Moss, Joel Hatinen, Peter Kus, Sahil Garg, Marta Mirolo, Ib Chorkendorff, Brian Seger, Jakub Drnec
Summary: We present a design for an electrochemical cell that can be used for High Energy X-ray operando studies of Membrane Electrode Assembly (MEA) based electrochemical systems. The flowplate materials in the cell can be changed according to experimental needs, allowing for the study of different chemistries and reactions. The design also enables the coupling of X-ray elastic scattering techniques with computed tomography reconstruction, which enables 3D mapping of chemical and structural properties in operating devices. The cell was originally designed and tested for studying CO2 electrolysis performance using Wide Angle X-ray Scattering (WAXS) technique.
JOURNAL OF POWER SOURCES
(2023)
Article
Instruments & Instrumentation
Clara C. Aletsee, Degenhart Hochfilzer, Anika Kwiatkowski, Markus Becherer, Jakob Kibsgaard, Ib Chorkendorff, Martin Tschurl, Ueli Heiz
Summary: Despite challenges in evaluating the catalytic performance of photoactive materials, a gas phase mu-photoreactor has been developed that is re-openable and re-usable, enabling post-characterization and catalyst screening studies. The reactor allows sensitive and time-resolved reaction monitoring at ambient pressure, and its microfabricated lid enhances sensitivity. The successful operation of the reactor is demonstrated through selective ethanol oxidation over Pt-loaded TiO2.
REVIEW OF SCIENTIFIC INSTRUMENTS
(2023)
Article
Chemistry, Physical
Degenhart Hochfilzer, Ib Chorkendorff, Jakob Kibsgaard
Summary: Working with non-noble electrocatalysts presents challenges in evaluating their intrinsic activity and characterizing their working state and changes. Despite numerous studies, these issues have not been adequately addressed, impeding significant progress. This Perspective discusses the pitfalls and challenges of working with non-noble-metal-based electrocatalysts, from synthesis to characterization, and proposes potential solutions. Reliable measurements of their intrinsic activity will enhance our understanding of electrocatalysis and facilitate the development of more active and selective electrocatalysts.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Asger B. Moss, Sahil Garg, Marta Mirolo, Carlos A. Giron Rodriguez, Roosa Ilvonen, Ib Chorkendorff, Jakub Drnec, Brian Seger
Summary: Membrane electrode assembly (MEA) CO2 electrolyzers are a promising approach for carbon-neutral chemical production, but stability issues due to flooding of the gas diffusion electrode (GDE) are common. This study investigates the causes of CO2 reduction reaction (CO2RR) selectivity suppression on Cu using in operando X-ray diffraction (XRD) analysis. The findings highlight the importance of proper ion management for enhanced durability in these devices.
Article
Chemistry, Multidisciplinary
Jon Bjarke Valbaek Mygind, Jakob B. Pedersen, Katja Li, Niklas H. Deissler, Mattia Saccoccio, Xianbiao Fu, Shaofeng Li, Rokas Sazinas, Suzanne Z. Andersen, Kasper Enemark-Rasmussen, Peter C. K. Vesborg, Jakob Doganli-Kibsgaard, Ib Chorkendorff
Summary: Ethanol plays a crucial role in the Li-NRR reaction, not only as a proton shuttle but also in facilitating a good solid-electrolyte interphase (SEI) and participating in electrolyte transformations. The ethanol-formed SEI enables ammonia synthesis even in an ethanol-free electrolyte.
Article
Chemistry, Physical
Xianbiao Fu, Valerie A. Niemann, Yuanyuan Zhou, Shaofeng Li, Ke Zhang, Jakob B. Pedersen, Mattia Saccoccio, Suzanne Z. Andersen, Kasper Enemark-Rasmussen, Peter Benedek, Aoni Xu, Niklas H. Deissler, Jon Bjarke Valbaek Mygind, Adam C. Nielander, Jakob Kibsgaard, Peter C. K. Vesborg, Jens K. Norskov, Thomas F. Jaramillo, Ib Chorkendorff
Summary: It has been discovered that calcium can mediate the reduction of nitrogen for ammonia synthesis in a lithium-free system. This finding offers the possibility of using abundant materials for the electrochemical production of ammonia, which is a critical chemical precursor and promising energy vector.
Article
Chemistry, Physical
Yu Qiao, Georg Kastlunger, Ryan C. Davis, Carlos Andreïs Giroïn Rodriguez, Andreas Vishart, Wanyu Deng, Qiucheng Xu, Shaofeng Li, Peter Benedek, Junjie Chen, Johanna Schro''der, Joseph Perryman, Dong Un Lee, Thomas F. Jaramillo, Ib Chorkendorff, Brian Seger
Summary: CO2 electrolysis converts CO2 into valuable fuels and chemicals, and adding Ag atoms to the Cu catalyst can modulate product preference. However, catalyst morphology, electrolyzer configuration, and reaction conditions strongly affect the synergistic effects and catalytic performance. This study prepared CuAg alloy catalysts and found that the interaction between Cu and Ag influenced the selectivity towards carbonyl production during CO2 reduction reaction.
Article
Chemistry, Physical
Ezra L. Clark, Rasmus Nielsen, Jakob Ejler Sorensen, Julius Lucas Needham, Brian Seger, Ib Chorkendorff
Summary: This paper investigates the effect of intermetallic alloying on the catalytic activity in electrochemical reactions. It is found that intermetallic phases allow for independent control over d-band energetics and work function, resulting in enhanced intrinsic activity for CO2 reduction. However, the propensity of these alloys to segregate in air poses a significant obstacle to studying their electrocatalytic activity.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Eric J. Mcshane, Valerie A. Niemann, Peter Benedek, Xianbiao Fu, Adam C. Nielander, Ib Chorkendorff, Thomas F. Jaramillo, Matteo Cargnello
Summary: In this study, the quantitative analysis of lithium alkoxide solid-electrolyte interphase (SEI) species and its effect on the efficiency of lithium-mediated electrochemical ammonia synthesis were investigated. The results showed that the thickness of the lithium alkoxide SEI layer significantly influenced the Faradaic efficiency, with an optimal thickness of around 4 μm.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Rasmus Nielsen, Tobias H. Hemmingsen, Tobias G. Bonczyk, Ole Hansen, Ib Chorkendorff, Peter C. K. Vesborg
Summary: This study presents a laser-annealing strategy for crystallizing selenium thin-films, improving their optoelectronic quality and providing a new approach for high-efficiency selenium solar cells.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Sahil Garg, Qiucheng Xu, Asger B. Moss, Marta Mirolo, Wanyu Deng, Ib Chorkendorff, Jakub Drnec, Brian Seger
Summary: Using operando wide-angle X-ray scattering, the formation of salt precipitates and their impact on the selectivity of CO2 reduction reaction and hydrogen evolution reaction were investigated. It was found that low-solubility salts can quickly precipitate over the catalyst layer, enhancing the hydrogen evolution reaction. On the other hand, highly soluble Cs salts prevent salt precipitation and flooding of the gas diffusion layer, improving the selectivity of CO2 reduction reaction. Furthermore, diluting cation concentration in the anolyte decreases salt precipitation and improves the selectivity of CO2 reduction reaction.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Hjalte Rorbech Ambjorner, Anton Simon Bjornlund, Tobias Georg Bonczyk, Edwin Dollekamp, Lau Morten Kaas, Sofie Colding-Fagerholt, Kristian Speranza Molhave, Christian Danvad Damsgaard, Stig Helveg, Peter Christian Kjaergaard Vesborg
Summary: Graphene is the thinnest imaginable membrane with high impermeability, but leakage pathways at the graphene-substrate interface compromise its impermeability. This study provides a kinetic analysis of interface-mediated leakage and shows that thermal processing can significantly improve the leak rate.