Article
Chemistry, Multidisciplinary
Valery Muravev, Jerome F. M. Simons, Alexander Parastaev, Marcel A. Verheijen, Job J. C. Struijs, Nikolay Kosinov, Emiel J. M. Hensen
Summary: This study unveiled the rich structural dynamics of a conventional catalyst during CO oxidation, confirming the presence of different active intermediates at different temperatures. The results highlight the importance of establishing structure-activity relationships for technical catalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Sai Luo, Xiaoguang Zhao, Yakun Qu, Lixin Wang, Bin Zhou, Wenzhe Si, Wei Fang
Summary: In this study, NAP-XPS was used to investigate the work function and element valence of the catalyst surface. Through DFT calculation, EELS, and specially designed O2-TPD characterization, it was demonstrated that generating oxygen vacancies led to a decrease in the average valence state of Mn elements from Mn4+ to less active Mn3+. Activity data of various VOCs suggest that generating a large number of oxygen vacancies could not enhance the activity of all types of VOC; for toluene oxidation, replenishing gas-phase oxygen into the bulk phase is also important. This work provides a novel way to explore the metal oxides' material exchange properties between its surface and gaseous oxygen and paves the way for the rational development of novel and versatile VOC oxidation catalysts.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
[Anonymous]
Summary: The dynamic behavior of ceria-supported Pd single atoms, clusters, and nanoparticles during CO oxidation was investigated using operando spectroscopy. The catalytic role of different Pd species was elucidated through a combination of in situ spectroscopy with transient and steady-state kinetic analysis, revealing that highly dispersed Pd-oxo species and interfacial Pd sites catalyze low-temperature CO oxidation, while metallic Pd contributes to the activity at elevated temperature.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Andrey V. Bukhtiyarov, Igor P. Prosvirin, Maxim A. Panafidin, Alexey Yu. Fedorov, Alexander Yu. Klyushin, Axel Knop-Gericke, Yan V. Zubavichus, Valery I. Bukhtiyarov
Summary: This study investigated the catalytic activity of HOPG-supported bimetallic Pd-Au catalysts towards CO oxidation by varying the Pd/Au atomic ratio. The results showed distinct differences in ignition temperatures and activity between catalysts with different initial Pd/Au atomic ratios.
Article
Chemistry, Physical
Chengfeng Zhu, Zhigang Chen, Wenbin Gong, Hao Li, Xuejian Liu, Xinxin Gan, Guang Yang, Jiangtao Di, Yi Cui
Summary: The study investigates the surface-reconstruction-accelerated OER activity of MoCoNi catalyst and finds that this catalyst exhibits excellent water electrolysis activity with low overpotential and small Tafel slope, as well as commercial RuO2-like stability. Using a vacuum-connected glove box and near ambient pressure X-ray photoelectron spectroscopy technology, subtle changes induced by potential and oxygen vacancies are directly detected, revealing the evolution of the electronic structure in the MoCoNi catalyst.
APPLIED SURFACE SCIENCE
(2022)
Article
Biochemistry & Molecular Biology
Xin Liu, Xin Zhang, Changgong Meng
Summary: The catalytic performance of single atom catalysts (SACs) in CO oxidation is found to be dependent on reaction conditions. At high temperatures, CO-mediated activation of O-2 and dissociation of peroxide intermediate is the dominant pathway, while at low temperatures and high CO partial pressures, coadsorbed CO-mediated dissociation of peroxide intermediate becomes plausible. Additionally, the presence of carbonate species benefits the conversion.
Article
Chemistry, Physical
Verena Pramhaas, Matteo Roiaz, Noemi Bosio, Manuel Corva, Christoph Rameshan, Erik Vesselli, Henrik Gronbeck, Guenther Rupprechter
Summary: Pt/ZrO2 model catalysts were prepared using ALD and studied through a combination of experimental techniques and theoretical calculations to understand CO adsorption and reaction processes. The researchers found that the onset of CO reaction depends on a delicate balance between CO disproportionation and oxidation, with initial CO oxidation being influenced by the removal of carbon deposits under current conditions.
Article
Materials Science, Multidisciplinary
Cheng Ding, Yue Chen, Jin Yang, Feifei Wang, Shibin Lu, Xing Li, Yuehua Dai
Summary: This study systematically investigates the interface characteristics, adsorption and migration behaviors of Ti metal on pristine and defective graphene intercalation. It is found that the presetting of single vacancy defect is the critical factor controlling ion penetration in the intercalation process.
MATERIALS TODAY COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Jiuxiang Dai, Zhongmiao Gong, Shitong Xu, Yi Cui, Meiyi Yao
Summary: Zirconium alloys are commonly used in the fabrication of nuclear fuel cladding due to their favorable properties. However, the initial oxidation behavior and the role of niobium in zirconium alloys are still challenging subjects.
ACTA PHYSICO-CHIMICA SINICA
(2022)
Article
Chemistry, Physical
Lin Zhu, Ali Al-Sakeeri, Filip Lenrick, Oskar Darselius Berg, Per Sjodin, Alexei A. Zakharov, Axel Knutsson, Anders Mikkelsen
Summary: The study investigates the changes in surface chemical composition and grain morphology of steel during vacuum brazing, revealing the variations in concentration and morphology of different elements at different temperatures and establishing a corresponding qualitative model.
SURFACE AND INTERFACE ANALYSIS
(2022)
Article
Chemistry, Physical
Tiancheng Pu, Adhika Setiawan, Bar Mosevitzky Lis, Minghui Zhu, Michael E. Ford, Srinivas Rangarajan, Israel E. Wachs
Summary: This study systematically investigates the nature of surface oxygen species on a silver powder catalyst and their reactivity with ethylene. The experimental results demonstrate that the silver surface is covered by a thin oxide layer during the oxidation treatment and ethylene oxidation process. It is found that Ag4-O2 is the active oxygen species on the oxidized silver surface.
Article
Chemistry, Physical
Liping Zhong, Mathias Barreau, Valerie Caps, Vasiliki Papaefthimiou, Michael Haevecker, Detre Teschner, Walid Baaziz, Elisa Borfecchia, Luca Braglia, Spyridon Zafeiratos
Summary: The addition of vanadium can stabilize the active state of cobalt, enhancing the activity and stability of the COPrOx reaction. The active sites are mainly composed of a cobalt-vanadate surface layer, with the presence of V5+ and Co2+ ions helping to inhibit carbonate species formation.
Article
Chemistry, Physical
Lianfeng Zhao, Weidi Cao, Yanjun Li, Endong Jin, Yanzhi Cai, Donghai Ding, Guoqing Xiao
Summary: Beta-SiAlON ceramics incorporated with h-BN were prepared by gel casting combined with reaction bonding procedure. The addition of h-BN improved the thermal shock resistance and oxidation resistance of the ceramics. The addition of h-BN facilitated the formation of a protective layer and inhibited the crystallization of the glassy phase, leading to a more stable protective layer and stagnating the oxidation process. The enhanced thermal shock resistance and oxidation resistance of beta-SiAlON with h-BN addition are of vital importance for applications in high temperature environments.
JOURNAL OF ALLOYS AND COMPOUNDS
(2023)
Article
Chemistry, Physical
Chengwu Qiu, Yaroslav Odarchenko, Qingwei Meng, Shaojun Xu, Ines Lezcano-Gonzalez, Paul Olalde-Velasco, Francesco Maccherozzi, Laura Zanetti-Domingues, Marisa Martin-Fernandez, Andrew M. Beale
Summary: The presence of surface oxygen vacancies (O-vac) on TiO2 can effectively reduce Co3O4 nanoparticles to CoO/Co-0. O-vac are particularly effective at reducing the edges of the nanoparticles, with smaller particles being more easily reduced than larger ones. During heating in H-2/syngas, further reduction and consumption of O-vac prevent the total reoxidation of Co nanoparticles, especially the smallest particles, thus maintaining the presence of metallic Co and potentially enhancing catalyst performance.
Article
Chemistry, Physical
Tuyet-Mai Tran-Thuy, Teng-Li Yu, Shawn D. Lin
Summary: This study investigates the influence of adsorbed H2O on CO oxidation over Au/BN catalysts. It is found that increasing the calcination temperature results in more Au particles distributed on the BN basal plane, increased water affinity, increased defects on BN, and altered CO oxidation activity. The turnover frequency is found to correlate with H2O physisorption, suggesting the involvement of (H2O)(n,ad) cluster in CO activation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Multidisciplinary Sciences
Zhiyu Yi, Le Lin, Yuan Chang, Xuda Luo, Junfeng Gao, Rentao Mu, Yanxiao Ning, Qiang Fu, Xinhe Bao
Summary: Dynamic control of oxide nanostructures is crucial for the design and understanding of oxide catalysts. This study demonstrates reversible conversion between Cr oxide nanoislands and clusters, highlighting the influence of redox treatments and environment.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Applied
Shiwen Li, Chao Wang, Caixia Meng, Yanxiao Ning, Guohui Zhang, Qiang Fu
Summary: This study explores the important processes of SEI formation and ion intercalation in rechargeable batteries under dynamic operating conditions, and finds that the choice of electrolyte significantly affects both processes, providing valuable strategies for the rational design and optimization of practical batteries in the future.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Physical
Caixia Meng, Feng Zhou, Hanqing Liu, Yuanyuan Zhu, Qiang Fu, Zhong-Shuai Wu
Summary: This study proposes a versatile strategy for boosting the capacitance of graphene-based planar micro-supercapacitors (MSCs) by using a highly concentrated water-in-salt ambipolar redox electrolyte. The results show significantly improved volumetric capacity, energy density, and long-term cycling stability compared to previous graphene-based MSCs. The good performance is attributed to the suppression of self-discharge by inhibiting the formation and diffusion of polyiodide ions.
ACS ENERGY LETTERS
(2022)
Article
Multidisciplinary Sciences
Yijing Liu, Rankun Zhang, Le Lin, Yichao Wang, Changping Liu, Rentao Mu, Qiang Fu
Summary: In this study, stripe-like MnO(001) and grid-like Mn3O4(001) monolayers were constructed on Pt(111) substrate to investigate hydrogen spillover. The experimental results showed that hydrogen diffused unidirectionally along the stripes on MnO(001), while it had an isotropic pathway on Mn3O4(001). The dynamic surface imaging in H-2 atmosphere revealed that hydrogen diffused 4 times faster on MnO than on Mn3O4, which was attributed to the one-dimensional surface-lattice-confinement effect. Theoretical calculations indicated that a uniform and medium O-O distance favored hydrogen diffusion while low-coordinate surface O atom inhibited it. This work illustrated the surface-lattice-confinement effect of oxide catalysts on hydrogen spillover and provided a promising route to improve the hydrogen spillover efficiency.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Yamei Fan, Fei Wang, Rongtan Li, Conghui Liu, Qiang Fu
Summary: In this study, gamma-alumina supports with different hydroxyl (OH) contents were prepared by calcinating pseudo-boehmite at different temperatures. The effect of surface OH on the oxidative redispersion process of supported Ag nanoparticles was investigated. The results show that the dispersion capacity of Ag species is thermodynamically determined by the surface OH contents, while the dispersion rate is kinetically limited by the OH densities. Both OH contents and OH densities play critical roles in the redispersion of metal particles and can be utilized to manipulate CO oxidation reactions catalyzed by Ag.
Article
Chemistry, Physical
Zhiyu Yi, Le Lin, Xuda Luo, Yanxiao Ning, Qiang Fu
Summary: Interfacial interaction between supported catalysts and the underlying substrate is crucial in catalysis. This study demonstrates that the interaction between Cr2O7 and Au can be weakened by applying an electric field, allowing for manipulation of the individual clusters. However, surface alloying with Cu enhances the interaction and makes the manipulation difficult.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Applied
Chao Wang, Xianjin Li, Guiming Zhong, Caixia Meng, Shiwen Li, Guohui Zhang, Yanxiao Ning, Xianfeng Li, Qiang Fu
Summary: In-depth understanding of the electrolyte-dependent intercalation chemistry in batteries is crucial for high-performance battery development. This study investigated the effect of electrolyte coordination structure on intercalation processes in the Al/graphite battery using operando XPS and X-ray diffraction. The weaker anion-cation interaction in the HMI-based electrolyte led to a lower atomic ratio of co-intercalated N to intercalated Al, resulting in lower ionic diffusion rate, capacity, and cycling performance. These findings emphasize the critical role of electrolyte coordination structure in (co-)intercalation chemistry.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Youwen Rong, Tianfu Liu, Jiaqi Sang, Rongtan Li, Pengfei Wei, Hefei Li, Aiyi Dong, Li Che, Qiang Fu, Dunfeng Gao, Guoxiong Wang
Summary: This study presents a strategy for highly selective production of acetate from CO electrolysis by constructing metal-organic interfaces. The Cu-organic interfaces constructed by in situ reconstruction of Cu complexes demonstrate impressive acetate selectivity, with high Faradaic efficiency and carbon selectivity. The study provides insights into the mechanism of selective acetate production.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Xuda Luo, Zhiyu Yi, Yanxiao Ning, Qiang Fu
Summary: This study investigates the structural evolution of supported metal catalysts under different treatment conditions. They construct model systems and use scanning tunneling microscopy and X-ray photoelectron spectroscopy to characterize the structural changes of supported Cu nanostructures. The results provide important insights for understanding the activity and stability of catalysts.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Yijing Liu, Le Lin, Liang Yu, Rentao Mu, Qiang Fu
Summary: The search for efficient non-noble-metal catalysts for selective oxidation reactions is important but often hampered due to controversial origin of the selectivity, especially for oxide-catalyzed reactions. In this study, high-pressure surface imaging techniques and theoretical calculations were used to identify spatially separated active sites for O-2 activation and H-2 adsorption on an ultrathin Mn3O4 surface, enabling selective oxidation of CO over H-2. The study sheds light on the atomic-level understanding of surface structure-dependent selective oxidation reactions on oxide catalysts.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Cui Dong, Rentao Mu, Rongtan Li, Jianyang Wang, Tongyuan Song, Zhenping Qu, Qiang Fu, Xinhe Bao
Summary: The interaction between oxide catalyst and oxide support is crucial in catalytic reactions. The construction of chemically bonded oxide-oxide interface by deposition of Co3O4 onto ZnO powder inhibits the complete reduction of Co3O4 and maintains a metastable CoOx state, resulting in high selectivity towards CO in CO2 hydrogenation reaction. On the other hand, physically contacted oxide-oxide interface formed by mechanical mixing promotes the reduction of Co3O4 and enhances CO2 conversion and selectivity towards CH4 through the remote spillover of dissociated hydrogen species.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Changping Liu, Le Lin, Hao Wu, Yijing Liu, Rentao Mu, Qiang Fu
Summary: Tuning the oxide/metal interface is crucial for enhancing the performance of many catalytic reactions. However, catalytic oxidation at the interface between non-reducible oxide and metal is challenging due to the reluctance of non-reducible oxides to lose oxygen. This study investigates CO oxidation at the ZnO/Au(111) interface using a ZnO monolayer film as an inverse catalyst and demonstrates that oxygen intercalation underneath the ZnO film significantly enhances the oxidation reaction.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Rongtan Li, Conghui Liu, Yamei Fan, Qiang Fu, Xinhe Bao
Summary: The activity of active oxygen species on supported Ag atoms can be effectively modulated by metal-support interactions using different oxide supports. The strong interaction between Ag and Al2O3 leads to the formation of more Ag-O-2(-) (superoxide) species, responsible for the selective oxidation of ethylene to ethylene oxide. The relatively weak interaction between Ag and SiO2 induces the generation of Ag-O (atomic oxygen) and Ag-O-2(2-) (peroxide) species, which are more active for complete oxidation of CO and ethylene to CO2. This work is of significance for deep understanding of active surface species in atomically dispersed metal catalysts.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Yamei Fan, Fei Wang, Rongtan Li, Conghui Liu, Qiang Fu
Summary: In this study, gamma-alumina supports with different OH contents were prepared by calcinating pseudo-boehmite at different temperatures. The role of surface OH groups in the oxidative redispersion of supported Ag nanoparticles was investigated. It was found that the dispersion capacity and rate of Ag species were determined by the surface OH contents and densities, respectively. These findings provide insights into the manipulation of Ag-catalyzed CO oxidation reaction.
Article
Chemistry, Multidisciplinary
Xuda Luo, Xiaoyuan Sun, Zhiyu Yi, Le Lin, Yanxiao Ning, Qiang Fu, Xinhe Bao
Summary: The rational design of highly stable and active metal catalysts requires a deep understanding of metal-support interactions at the atomic scale. Ultrathin films of FeO and FeO2-x grown on Pt(111) were used as templates for the construction of well-defined metal nanoclusters. The selective nucleation and formation of Cu clusters were driven by different interactions with the Fe oxide domains, which were validated by density functional theory calculations. The study reveals that the reactivity descriptor of surface O atoms determines the interaction between metal adatoms and Fe oxides, providing guidance for the rational design of supported single-atom and nanocluster catalysts.
