Article
Engineering, Environmental
Peng Rao, Yalin Liu, Ya-Qiong Su, Mingjun Zhong, Kun Zhang, Junming Luo, Jing Li, Chunman Jia, Yijun Shen, Chong Shen, Xinlong Tian
Summary: This study developed a unique 3D core-shell nanostructure bifunctional oxygen catalyst with excellent electrocatalytic performance and stability, showing promising applications in metal-air batteries.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Jingjing Zhang, Fumin Tang, Kechuang Wan, Yange Yang, Cunman Zhang, Ping Wen Ming, Bing Li
Summary: In this study, CoFe alloy nanoparticles encapsulated in N,O co-doped multilayer graphitized shells were used as effective bifunctional catalysts for zinc-air batteries. The resulting heteroatom-doped carbon highly graphitized bimetallic catalysts showed high durability and the homemade zinc-air battery exhibited high power density and high specific capacity with excellent stability during battery cycling processes.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Physical
Haifang Xie, Dahai Zeng, Bing Du, Peng Zhang, Huaijun Lin, Qingyang Li, Zhidan Lin, Wei Li, Yuying Meng
Summary: This study reports a novel Co2P@NOCs non-precious metal electrocatalyst that can serve as an excellent noble metal-free bifunctional electrocatalyst for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) in alkaline media. The Co2P@NOC-2 electrocatalyst exhibits low overpotential and a small Tafel slope for OER, as well as positive onset and half-wave potentials for ORR. It also demonstrates better methanol tolerance and long-term durability compared to the commercial Pt/C catalyst.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Nanping Deng, Qiang Zeng, Yang Feng, Hongjing Gao, Gang Wang, Jing Yan, Tinglu Zheng, Yong Liu, Weimin Kang, Bowen Cheng
Summary: The study developed a strategy to prepare CoP nanoparticles embedded in three-dimensional porous network-like structured N, O co-doped carbon nanofibers. The resulting material showed enhanced ORR/OER activity and was used as a bi-functional electrocatalyst in rechargeable zinc-air batteries. The zinc-air battery with the CoP@N, O co-doped PCNF catalyst exhibited high specific capacity and energy density, and stable cycling performance.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Xinlei Luo, Ziheng Zheng, Bingxue Hou, Xianpan Xie, Cheng Cheng Wang
Summary: A novel catalyst derived from the pyrolysis of a Co/Fe/Zn zeolitic imidazolite framework shows promising oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activity. The Co-N-C-900 catalyst exhibits E-1/2 = 0.854 V and E-j=10 = 1.780 V. A rechargeable Zn-air battery equipped with the Co-N-C-900 cathode catalyst demonstrates a high peak power density of 275 mW cm(-2), outperforming commercial 20% Pt/C. Importantly, the designed Zn-air battery with the Co-N-C-900 catalyst exhibits good cycling stability for 180 h.
Article
Chemistry, Inorganic & Nuclear
Tao Meng, Baoguang Mao, Minhua Cao
Summary: The coupling of dual active components into an integrated catalyst and understanding their electronic interaction behavior is crucial for achieving high energy-conversion efficiency in Zn-air batteries. The MnO/Co@NGC catalyst demonstrated excellent bifunctional ORR/OER activity with a small overpotential gap, providing high trip efficiency and cycling stability for ZABs. This study not only provides a promising approach for developing advanced energy-related materials, but also highlights the importance of interfacial charge distribution in oxygen electrocatalysis.
INORGANIC CHEMISTRY
(2021)
Article
Energy & Fuels
Shaojie Shi, Biaolong Wang, Yifei Wang, Yanmin Yang, Zhiguo Zhang, Yousheng Xu, Yange Suo
Summary: The rational design and preparation of bifunctional electrocatalysts with high catalytic performance for both ORR and OER are crucial for the development of fuel cells and regenerative metal-air cells. In this work, a simple compound-assisted pyrolyzing strategy is reported to synthesize Co-N-C materials by high-temperature annealing of ZIF-12, and the results demonstrate the importance of optimal pore structure, higher carbon defect content, and higher Co-N-x concentration for improving the electrochemical performances of the Co-N-C catalysts.
Article
Chemistry, Physical
Fengyue Sun, Lingyu Yang, Changle Yue, Yang Liu, Wenjing Bao, Yongxiao Tuo, Xiang Feng, Yukun Lu
Summary: This study utilized Strandberg-type polyoxometalate as pre-assembled molecular platforms to construct and regulate NiMoS active sites at the atomic level. O,P doping was performed to boost the number of active sites using a controllable sulfidation method, resulting in O,P-NiMoS nanoparticles with significant catalytic activity. This research provides a feasible strategy for the rational design of efficient electrocatalysts for renewable energy applications.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Energy & Fuels
Qingtao Wang, Kai Cui, Dongxu Liu, Yanxia Wu, Shufang Ren
Summary: This article describes a method for synthesizing a non-noble metal catalyst and demonstrates its high efficiency and excellent stability in the hydrogen evolution reaction and oxygen evolution reaction. Through in situ growth and annealing, nitrogen atoms on the catalyst surface can form more catalytic active sites, and the use of carbon nanosheets as a matrix can improve the electrochemical performance of the composite.
Article
Chemistry, Inorganic & Nuclear
Ting Li, Fei Gu, Xiao Hui Chen, Qing Zhang, Hong Chuan Fu, Hong Qun Luo, Nian Bing Li
Summary: A 2D/3D hierarchical electrocatalyst, Co(OH)2-CeO2/Co, consisting of Co(OH)2-CeO2 nanosheet-decorated Co dendrites, is proposed. The electronic structure of the Co site is optimized through the strong electronic interaction of the Co(OH)2-CeO2 heterojunction, facilitating intermediates adsorption and H2O dissociation. The open 2D/3D structure formed by introducing the Co substrate reduces nanosheet accumulation and promotes electrolyte diffusion, improving active site utilization and electron transfer pathway.
INORGANIC CHEMISTRY
(2023)
Review
Chemistry, Physical
Daniel A. Kurtz, Bryan M. Hunter
Summary: Transition metal oxides/oxyhydroxides have generated much interest as electrocatalysts for water splitting due to their ability to cycle between different oxidation states. A thermodynamic model is proposed to explain the trends in first-row transition metal catalysts for oxygen evolution half-reaction. The model can provide quantitative predictions based on experimental data.
Article
Multidisciplinary Sciences
Jun Xu, Huanyu Jin, Teng Lu, Junsheng Li, Yun Liu, Kenneth Davey, Yao Zheng, Shi-Zhang Qiao
Summary: The trade-off between activity and stability of oxygen evolution reaction (OER) catalysts in proton exchange membrane water electrolyzer (PEMWE) is challenging. We combine the advantages of crystalline IrO2 and amorphous IrOx to form a lattice water-incorporated iridium oxide (IrOx center dot nH(2)O) with a hollandite-like framework structure. This material exhibits boosted activity and ultrahigh stability, with a stability number of 1.9 x 10^7 noxygen nIr^-1. The lattice water-assisted modified OER mechanism contributes to improved activity and concurrent stability in the PEMWE.
Article
Chemistry, Physical
Zhi Xie, Qiaoling Li, Xingkai Peng, Xuewei Wang, Lingli Guo, Xinghua Zhang, Zunming Lu, Xiaojing Yang, Xiaofei Yu, Lanlan Li
Summary: The study synthesized B/N co-doped porous carbon shell-encapsulated Fe2N nanoparticles as a highly efficient and durable catalyst for ORR. The introduction of B dopant improved N element doping, amended the carbon shell, and enhanced electron transfer efficiency from Fe2N NPs to the carbon surface.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Jianbo Zhao, Xiaomeng Li, Meng Zhang, Zhuo Xu, Xiaomei Qin, Yingfan Liu, Lifeng Han, Gao Li
Summary: In this study, a hollow mesoporous Co-N-C@mSiO(2) nanostructure derived from ZIF-67 was designed via the encapsulation-pyrolysis strategy. The Co-N-C@mSiO(2) catalyst exhibited excellent catalytic performance in the furfural hydrogenation towards furfuryl alcohol with good stability, and it was much better than other reported transition metal catalysts. This work provides a novel and facile strategy for preparing highly efficient non-precious metal catalysts to replace Cr-based and noble metal catalysts for furfural hydrogenation.
Article
Chemistry, Multidisciplinary
Xiaoqing Lu, Jiao Li, Shoufu Cao, Yuying Hu, Chunyu Yang, Zengxuan Chen, Shuxian Wei, Siyuan Liu, Zhaojie Wang
Summary: This study investigates the effect of introducing S or P atoms into N coordination on the electronic structure and catalytic performance of FeN4 SACs. It demonstrates that FePN3 can effectively activate O-2 and promote ORR, while FeSN3 is beneficial to H2O activation and OER. Both FePN3 and FeSN3 exhibit outstanding stability. The N,P and N,S co-coordination provides a better catalytic environment for SACs in ORR and OER.
Article
Chemistry, Physical
Romain Tort, Olivia Westhead, Matthew Spry, Bethan J. V. Davies, Mary P. Ryan, Maria-Magdalena Titirici, Ifan E. L. Stephens
Summary: The performance of Li-mediated ammonia synthesis has improved significantly since its reintroduction, but the fundamental understanding of this reaction has been slower due to uncontrolled variables. To address this, a nonaqueous LiFePO4 reference electrode was developed, providing a redox anchor for measuring potentials and estimating energy efficiency loss. The relationship between partial current density and potentials was uncovered using this reference, suggesting that only the electrochemical step of lithium plating is involved in the process. The LiFePO4/Li+ equilibrium was also used to probe Li-ion activity changes in situ. The aim is to promote a better understanding of this reaction by developing more defined systems.
ACS ENERGY LETTERS
(2023)
Review
Chemistry, Multidisciplinary
Olivia Westhead, Jesus Barrio, Alexander Bagger, James W. Murray, Jan Rossmeisl, Maria-Magdalena Titirici, Rhodri Jervis, Andrea Fantuzzi, Andrew Ashley, Ifan E. L. Stephens
Summary: This Review provides a coherent comparison of recent progress made in dinitrogen fixation on solid electrodes, homogeneous catalysts, and nitrogenases. By establishing the cross-cutting themes and synergies between these systems, we identify viable avenues for future research.
NATURE REVIEWS CHEMISTRY
(2023)
Article
Energy & Fuels
Carla de Tomas, Sarat Alabidun, Luke Chater, Matthew T. Darby, Federico Raffone, Paolo Restuccia, Heather Au, Magda M. Titirici, Clotilde S. Cucinotta, Maria Crespo-Ribadenyra
Summary: In this study, the effect of sulfur doping on hard carbon anodes for sodium-ion batteries is investigated using a combination of experiments and theory. The hard carbons are synthesized through a two-step process and subsequent sulfur doping is introduced via chemical-vapour deposition. The sulfur-doped hard carbon exhibits enhanced sodium storage capacity and improved cycling reversibility, which is attributed to the increased sodium adsorption energies and facilitated sodium desorption due to the sulfur chemisorbed onto the hard carbon. This study provides insights into the mechanism and opens up possibilities for more efficient sodium-ion batteries.
JOURNAL OF PHYSICS-ENERGY
(2023)
Article
Engineering, Environmental
Feng Li, Zhenyu Guo, Ziqing Song, Lili Wang, Lituo Zheng, Gang Cheng, Cecilia Mattevi, Zhensheng Hong, Maria-Magdalena Titirici
Summary: We present a new method for synthesizing high-crystallinity graphite at a low temperature of 1100 degrees C in just 13 minutes. This sustainable and cost-effective method utilizes a multi-physics field coupling with a Ni catalyst, and shows exceptional kinetics and accelerated breaking of C-O bonds. The synthesized graphite exhibits excellent performance in Li+ storage and Na-ion batteries, indicating its potential in energy storage applications.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Zhenyu Guo, Zhen Xu, Fei Xie, Jinglin Jiang, Kaitian Zheng, Sarat Alabidun, Maria Crespo-Ribadeneyra, Yong-Sheng Hu, Heather Au, Maria-Magdalena Titirici
Summary: Emerging sodium-ion batteries (NIBs) and potassium-ion batteries (KIBs) have the potential to complement lithium-ion battery (LIBs) technology and diversify the battery market. Hard carbon synthesized by hydrothermal carbonization and subsequent pyrolysis at different temperatures exhibits different ion-storage trends and shows promise as sustainable and scalable anodes for beyond Li-batteries. The best-performing hard carbon material achieves excellent energy/power densities and stable long-term cycling performance in a Na-ion pouch cell.
ADVANCED MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Silvia Favero, Ifan E. L. Stephens, Maria-Magdalena Titirci
Summary: Alkaline-based electrochemical devices, such as anion exchange membrane (AEM) fuel cells and electrolyzers, are gaining attention as emerging decarbonization technologies. The anion exchange ionomer, a crucial component in these devices, has a significant impact on the mechanical integrity, morphology, activity, and stability of the catalyst layer. This review provides an overview of the current state, requirements, and remaining challenges of this ionomer in the context of AEM electrolyzers and fuel cells.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zamaan Mukadam, Sihang Liu, Angus Pedersen, Jesus Barrio, Sarah Fearn, Saurav Ch. Sarma, Maria-Magdalena Titirici, Soren B. Scott, Ifan E. L. Stephens, Karen Chan, Stefano Mezzavilla
Summary: In this study, Cu and Co single-atom catalysts supported on carbon electrodes were used to investigate the electrochemical reduction of furfural, a biomass-derived chemical. Under mild conditions, hydrofuroin, a valuable precursor to sustainable jet fuels, was selectively produced. The study also revealed insights into the mechanism and stability of the catalysts and provided a blueprint for catalyst design in this reaction.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
O. Westhead, R. Tort, M. Spry, J. Rietbrock, R. Jervis, A. Grimaud, A. Bagger, I. E. L. Stephens
Summary: The verification of the lithium-mediated nitrogen reduction system in 2019 has resulted in an increase in literature on improving the faradaic efficiency, stability, and activity. However, accurately quantifying the overpotential and analyzing voltage losses has been challenging. This study presents a simple method for determining the Reversible Hydrogen Electrode potential in the system and identifies sources of potential losses. The observed minimum overpotential was -3.59 +/- 0.07 V vs. RHE, with a faradaic efficiency of 6.5 +/- 0.2%.
FARADAY DISCUSSIONS
(2023)
Review
Chemistry, Physical
Hans Becker, James Murawski, Dipak V. Shinde, Ifan E. L. Stephens, Gareth Hinds, Graham Smith
Summary: Low temperature water electrolysers are sensitive to water quality and common impurities can affect the device performance and lifetime. Purifying the feed water adds cost and complexity, and failure of purification equipment can cause degradation of the electrolysers. This review provides a comprehensive overview of impurities in operating electrolysers, including their sources, degradation mechanisms, characterization techniques, water purification technologies, and mitigation strategies. It generalizes existing mechanisms, proposes new ones, and offers a framework for considering operational implications.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Chemistry, Physical
Michael P. Mercer, Mangayarkarasi Nagarathinam, E. Maximiliano Gavilan-Arriazu, Anshika Binjrajka, Swoyam Panda, Heather Au, Maria Crespo-Ribadeneyra, Maria-Magdalena Titirici, Ezequiel P. M. Leiva, Harry E. Hoster
Summary: Hard carbons have potential as anode materials in sodium-ion battery technologies. Understanding the driving forces of sodium insertion into hard carbons, particularly into nanopores, is crucial for material optimization. By using entropy profiling, researchers were able to determine the onset of nanopore filling and quantify the energetics of sodium inside the nanopores, providing insights for tuning the cell cut-off voltage.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Angus Pedersen, Jinil Pandya, Grazia Leonzio, Alexey Serov, Andrea Bernardi, Ifan E. L. Stephens, Maria-Magdalena Titirici, Camille Petit, Benoit Chachuat
Summary: This study compares the environmental impacts and economic analysis of using non-Pt-based electrocatalyst Fe-N-C to replace Pt/C in PEMFCs. The findings show that Fe-N-C can reduce environmental damages and human health impacts, but it still faces issues such as electricity consumption and resource depletion. The cost of PEMFC stacks with Fe-N-C cathode would increase compared to those with Pt/C cathode due to the increase in environmental externalities. Continued improvement of Fe-N-C performance is necessary to replace Pt-based cathode catalysts in PEMFCs.
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)