Article
Chemistry, Physical
Haifeng Yuan, Lili Zhao, Bin Chang, Yuke Chen, Tianjiao Dong, Jietong He, Di Jiang, Wanqiang Yu, Hong Liu, Weijia Zhou
Summary: In this study, efficient electrocatalysts for hydrogen evolution reaction (HER) were synthesized by laser ablation and reduction, resulting in Mo2C micropillars decorated with Pt nanoparticles. These catalysts showed excellent performance and stability in acid media. Integrated gas diffusion and catalytic electrodes constructed using laser technology exhibited lower voltage in a proton exchange membrane water electrolyzer compared to traditional catalysts, offering promising applications in the field of hydrogen energy.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Organic
Qinglong Zhou, Jiaomeng Li, Tianyi Wang, Xing Yang
Summary: This article presents a practical and efficient base-mediated sulfur arylation reaction for the preparation of sulfilimines. By using various N-acyl and N-aryl sulfenamides, and diaryliodonium salts as reactants, the sulfilimines can be obtained in high yields with excellent chemoselectivities.
Article
Materials Science, Multidisciplinary
Jagan Radhakrishnan, Krishnendu Biswas
Summary: In this study, tin sulfide nanomaterials including SnS, SnS2, and Sn2S3 were successfully synthesized via a one-step method. The ballmilled SnS and Sn2S3 samples exhibited enhanced electrocatalytic HER activity, which can be attributed to the increase of exposed catalytic active sites.
MATERIALS SCIENCE AND ENGINEERING B-ADVANCED FUNCTIONAL SOLID-STATE MATERIALS
(2023)
Article
Chemistry, Physical
Jyoti Ranjan Mandal, Khushboo Singh, Vinod K. Shahi
Summary: A bifunctional electrocatalyst loaded on an amphoteric ion exchange membrane was developed for efficient water splitting and simultaneous HER and OER processes in alkaline media. The prepared membrane electrode assembly exhibited better overall water splitting performance compared to other commercialized membrane substrates and reported electrocatalysts.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Physical
Wei Song, Zhe Fu, Pengfei Ma, Xiao Liu, Yongliang Guo, Ling Fu, Chaozheng He
Summary: NH3 is a valuable chemical in agriculture and industry due to its high hydrogen capacity and energy density. However, current industrial-scale NH3 synthesis processes consume large amounts of energy and cause pollution. This study presents a new strategy for the production of NH3 using electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions. Single-atom catalysts of noble metal (Ru, Rh, Pd, Os, Ir, Pt) atoms anchored on non-metallic atom (B, N, O)-doped graphyne were designed and their effects on NRR performance were investigated through density functional theory calculations. The result showed that RuB@GY and OsB@GY exhibited the highest NRR performance and could effectively inhibit competing hydrogen evolution reactions.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Simonas Ramanavicius, Carla Bittencourt, Arnas Naujokaitis, Vidas Pakstas, Arunas Jagminas
Summary: By synthesizing a novel material composed of strontium molybdate mixed with molybdenum disulfide, the number of active sites in MoS2 materials can be significantly increased, enhancing the catalytic activity and stability for hydrogen evolution reaction. Compared to pure synthetic MoS2, this hybrid material demonstrates superior performance in terms of surface catalytic activity and stability.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Multidisciplinary
Fangfang Wang, Kuanjian Zhang, Shifeng Li, Qingqing Zha, Yonghong Ni
Summary: In this study, W-doped α-Ni(OH)2 honeycomb-like microstructures were successfully fabricated, demonstrating excellent OER electrocatalytic performance. The sample deposited at -100 mA cm(-2) for 15 minutes showed the strongest OER electrocatalytic capability.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Materials Science, Multidisciplinary
Alireza Kokabi, Mina Fayazi
Summary: The noble metal atoms decorated over the porous monolayer of C8N8 exhibit superior performance in the reduction reaction of low-density environmental NO gas, with osmium atom being the most energetically favored catalyst. Both nitrogen-and carbon-dominated large rings can adsorb noble metal atoms, but no clustering occurs on pristine C8N8.
MATERIALS TODAY COMMUNICATIONS
(2023)
Review
Chemistry, Physical
Rameez Ahmad Mir, Sanjay Upadhyay, O. P. Pandey
Summary: In this paper, the environmental issues and energy crisis caused by the overuse of fossil fuels are discussed. The importance of renewable and non-carbon emission energy sources, particularly hydrogen generated through electrochemical water splitting, is emphasized. The need for low-cost and efficient electrocatalysts for hydrogen evolution reaction (HER) is introduced, with a focus on nano transition metal carbides (TMCs) such as molybdenum carbide (Mo2C). The progress and advances in improving the electrocatalytic performance of nano Mo2C are presented, including synthesis, size, shape, and carbon support. The role of different carbon species and nitrogen doping in enhancing the HER activity over Mo2C are also discussed.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Mingming Guo, Mingjuan Ji, Wei Cui
Summary: Multifunctional catalysts are crucial for the development of electrochemical energy systems. Single metal atoms embedded in a two-dimensional substrate, such as graphyne, have shown great potential as outstanding catalysts. This study used density functional theory simulations to identify promising codecorated graphyne materials and established a quantitative structure-property relationship between electronic density of states structure and catalytic performance.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Liang Yuan, Yingmeng Zhang, Jinhong Chen, Yongliang Li, Xiangzhong Ren, Peixin Zhang, Liwei Liu, Jinxiang Zhang, Lingna Sun
Summary: In this study, a novel MoS2@CoSe2-CC hybrid was synthesized as an efficient HER electrocatalyst via a simple hydrothermal reaction. The hybrid exhibited a three-dimensional hierarchical structure, providing more active sites and excellent structural stability. It showed outstanding catalytic performance in alkaline media with a small Tafel slope and low HER overpotential.
Article
Chemistry, Physical
Carlos V. M. Inocencio, Julie Rousseau, Nadia Guignard, Christine Canaff, Sophie Morisset, Teko W. Napporn, Claudia Morais, K. Boniface Kokoh
Summary: Transition metal sulfides (NiSx, MoSx and Ni0.5Mo0.5Sx) were synthesized and their HER performance was evaluated. The presence of nickel oxide on the surface of Ni0.5Mo0.5Sx was found to enhance water dissociation, while molybdenum sulfide catalyzed the reduction of adsorbed hydrogen species. When mixed with Carbon Vulcan, Ni0.5Mo0.5Sx showed a slightly higher overpotential compared to 40% Pt/C.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Sangeetha Kumaravel, Dhirendra Kumar, Selvasundarasekar Sam Sankar, Arun Karmakar, Ragunath Madhu, Krishnendu Bera, Hariharan N. Dhandapani, Sreenivasan Nagappan, Sudip Chakraborty, Subrata Kundu
Summary: An advanced vacancy-rich bi-chalcogenide, Cu2S-Se@Cu, was developed as a highly efficient catalyst for HER in acid. The catalyst exhibited a small overpotential and a low Tafel slope. Density functional theory studies revealed that Cu2S-Se over the Cu surface reduced the band gap and enhanced the catalytic activity.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Fengjiao Quan, Guangming Zhan, Pengfei Xu, Wenjuan Shen, Falong Jia, Lizhi Zhang, Jianfen Li
Summary: The study proposes a maximum orbital overlapping strategy to select suitable transition metal catalysts for the electrocatalytic nitrogen reduction reaction (ENRR). By introducing La single-atom catalysts onto the surface of few-layer MoS2, the Faradaic efficiency of NH3 was greatly improved to 18.2%.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Xiaohao Jiang, Rongtao Xiao, Honggui Wang, Ya Zhang
Summary: Hydrogen, as a high calorific and zero carbon energy source, has gained significant attention in recent years. In this study, amorphous molybdenum sulfide was uniformly wrapped around the surface of Ni9S8/NF nanowires to obtain a-MoSX@Ni9S8/NF nanoflower rods. The composite exhibited a low overpotential and high electrochemically active surface area, achieving efficient hydrogen evolution reaction (HER) with the assistance of an external thermal field. The a-MoSX@Ni9S8/NF showed excellent hydrogen precipitation performance under 80 degrees C and maintained good reproducibility and durability after 5000 cycles in acidic media. The Faraday efficiency of the composite reached 92.6%.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Physical
Neha Neha, Thibault Rafaideen, Theo Faverge, Frederic Maillard, Marian Chatenet, Christophe Coutanceau
Summary: In this study, the electrooxidation of glucose on gold and platinum nanoparticles in alkaline medium was investigated. It was found that glucose can adsorb on both surfaces at low potentials, but the adsorbed species were different. On platinum nanoparticles, glucose adsorption and hydrogen atoms oxidation into protons occurred in the first oxidation peak, while the oxidation of glucose into lactone and gluconate and of adsorbed carbon monoxide into carbon dioxide happened in the second electrochemical feature. For gold nanoparticles, adsorbed hydrogen atoms were transformed into molecular hydrogen, and glucose was adsorbed as gluconate species.
Article
Chemistry, Physical
Raphael Chattot, Marta Mirolo, Isaac Martens, Kavita Kumar, Vincent Martin, Amir Gasmi, Laetitia Dubau, Frederic Maillard, Luis Castanheira, Jakub Drnec
Summary: Efficient testing of PEMFC cathode catalysts' long-term stability requires the use of accelerated stress tests and auxiliary in situ electro-chemical characterization techniques such as cyclic voltammetry. This study reveals that the cyclic voltammetry experiment performed at the end of the AST controls the increase of the coherent domain size monitored on the aged catalyst.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Hongxin Ge, Nicolas Bibent, Keyla Teixeira Santos, Kavita Kumar, Julien Jaxel, Moulay-Tahar Sougrati, Andrea Zitolo, Marc Dupont, Frederic Lecoeur, Michel Mermoux, Vincent Martin, Laetitia Dubau, Frederic Jaouen, Frederic Maillard, Sandrine Berthon-Fabry
Summary: A series of Fe-NC aerogel catalysts were synthesized by modulating the nitrogen source and texture, and the importance of nitrogen sources in stabilizing Fe atoms and forming active sites was revealed. The mass activity of the catalysts exhibited a linear relationship with Fe content and reached 3.0 A g(-1) in 0.05 M H2SO4 and RDE setup. The performance in PEMFC showed the same tendency and was not affected by low mesopore volume.
Article
Chemistry, Physical
Viktoriia A. Saveleva, Kavita Kumar, Pascal Theis, Nicole Segura Salas, Ulrike I. Kramm, Frederic Jaouen, Frederic Maillard, Pieter Glatzel
Summary: This study investigates the structural composition of Fe-N-C materials for the oxygen reduction reaction in proton-exchange membrane fuel cells, before and after catalyst layer preparation, using X-ray absorption and emission spectroscopies. The results reveal the significant impact of the preparation step on the electronic structure and local coordination of Fe, emphasizing the importance of determining the Fe-N-C catalyst structure in the prepared electrode for further studies of the structure-activity-stability correlations.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Secil Unsal, Robin Girod, Christian Appel, Dmitry Karpov, Michel Mermoux, Frederic Maillard, Viktoriia A. Saveleva, Vasiliki Tileli, Thomas J. Schmidt, Juan Herranz
Summary: Non-noble metal catalysts (NNMCs) have the potential to replace expensive Pt-based materials in proton exchange membrane fuel cells (PEMFCs), but their poor durability hinders their commercial implementation. The degradation mechanisms include operative demetallation, electro-oxidation of the carbonaceous matrix, and chemical degradation caused by H2O2 radicals. However, the relative contributions of these mechanisms to overall performance loss are not well understood. In this study, degradation protocols were used to determine that H2O2-related instability is dependent on the ORR charge, while electro-oxidation of the carbon matrix at high potentials is more detrimental to NNMCs' activity than demetallation at low potentials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Theo Faverge, Bruno Gilles, Antoine Bonnefont, Frederic Maillard, Christophe Coutanceau, Marian Chatenet
Summary: The oxidation mechanisms of glucose, gluconic acid, and sorbitol on gold, platinum, and palladium surfaces were studied using cyclic voltammetry, differential electrochemical mass spectrometry, and in situ Fourier transform infrared spectroscopy. The nature of the reactant influenced the onset of the oxidation reaction, with glucose being oxidized at low potentials on all three surfaces, while gluconic acid and sorbitol exhibited poisoning effects. The metal surface also influenced the reaction pathways, with glucose oxidation being initiated through the partial dissociative adsorption of glucose on all three surfaces. Gold demonstrated the highest activity, selectivity, and specificity for glucose oxidation to gluconate at low potentials. The study reveals a reactant, catalyst, and potential-dependent mechanism.
Review
Chemistry, Multidisciplinary
Kavita Kumar, Laetitia Dubau, Frederic Jaouen, Frederic Maillard
Summary: One bottleneck in the widespread use of fuel cell vehicles, especially PEMFCs, is the high cost of the cathode due to the need for precious metals as catalysts. Short-term solutions involve improving platinum utilization, while long-term solutions involve developing catalysts based on Earth-abundant elements. The degradation mechanisms of Metal-N-C electrocatalysts in the acidic environment of PEMFCs are an important research topic, with recent advances in understanding its mechanisms and mitigation approaches.
Article
Chemistry, Physical
Viktoriia A. A. Saveleva, Marius Retegan, Kavita Kumar, Frederic Maillard, Pieter Glatzel
Summary: Researchers used VtC XES technique to characterize the Fe-N-C catalyst and found that the local geometry of Fe atoms changed after stress tests.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Theo Faverge, Bruno Gilles, Antoine Bonnefont, Frederic Maillard, Christophe Coutanceau, Marian Chatenet
Summary: The mechanisms of oxidation of glucose, gluconic acid, and sorbitol on gold, platinum, and palladium are investigated using cyclic voltammetry, differential electrochemical mass spectrometry, and in situ Fourier transform infrared spectroscopy. The nature of the reactant significantly influences the onset of the oxidation reaction, with glucose's anomeric function oxidized at low potentials on all three surfaces, while gluconic acid and sorbitol poison the surface at low potentials. Different reaction pathways are observed based on the metal surface, and gold features the best activity, selectivity, and specificity for glucose oxidation into gluconate at low potentials. The study highlights the dependence of the mechanism on reactant, catalyst, and potential.
Article
Chemistry, Physical
Angus Pedersen, Alexander Bagger, Jesus Barrio, Frederic Maillard, Ifan E. L. Stephens, Maria-Magdalena Titirici
Summary: Proton exchange membrane fuel cells need to reduce construction costs to improve commercial viability, which can be achieved by eliminating platinum and using single metal atoms coordinated to nitrogen-doped carbon (M-N-C) as alternative electrocatalysts for O-2 reduction. In the past decade, significant progress has been made in the synthesis, characterization, and electrocatalytic performance of M-N-Cs. This Perspective article provides a review of the important achievements in the last decade, discusses current gaps in knowledge, and suggests future research directions. Additionally, it presents a new outlook on M-N-C stability and atomistic understanding using density functional theory simulations.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
