Article
Chemistry, Physical
Dong Liu, Feiyang Hu, Yue Yan, Runping Ye, Xiaohan Chen, Bingying Han, Zhang-Hui Lu, Li Zhou, Gang Feng, Rongbin Zhang
Summary: By using a three-dimensional ordered microporous material, Au/CeO2 catalyst was synthesized and showed complete CO oxidation at lower temperatures compared to traditional catalysts. This microporous catalyst also exhibited good stability and the promotion of metal distribution and oxygen vacancies by the fiber structure was discovered through various characterizations.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Yanling Li, Jinfu Ma, Shaolin Yang, Lihua Cui, Hui Lu
Summary: Material defects, specifically oxygen vacancies, play a crucial role in high electron conductivity and surface property adjustment in metal oxide-based supercapacitors. The novel Co(OH)(2)/SnO./C hybrid nanosheets synthesized in this study exhibit high specific capacitance and good cycle stability, showing potential for use in energy storage applications.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Nanoscience & Nanotechnology
Junnan Chen, Yujie Qi, Ming Lu, Shaoming Dong, Bingsen Zhang
Summary: In this study, the interface microstructures of Pt/TiO2 catalysts were characterized using electronic energy loss spectroscopy. The presence of TiOx coating on the surface of Pt metal particles was observed after high-temperature reduction processing. A quantitative analysis method based on Gaussian function fitting was established to determine the stoichiometric number of TiOx phases. The origins of TiOx and its effects on the electronic structure of the material were discussed and analyzed using density functional theory calculations.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Review
Chemistry, Physical
Haotian Zhang, Siyuan Fang, Yun Hang Hu
Summary: Single-atom catalysts (SACs) have attracted significant attention due to their high atom utilization and excellent catalytic activities. This review discusses the design principles, synthesis methods, and the influence of metal-support interactions on the activity of SACs for CO oxidation. Moreover, the CO oxidation mechanisms over SACs are evaluated and the future research directions and challenges for SAC-catalyzed CO oxidation are outlined.
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING
(2022)
Article
Chemistry, Physical
Miao He, Yueqiang Cao, Jian Ji, Kai Li, Haibao Huang
Summary: By modulating the metal-support interaction and utilizing oxygen vacancies, this study successfully demonstrated the catalytic oxidation of formaldehyde at room temperature using reduced TiO2 as a support for Pd nanoparticles. The synergy between the metal-support interaction and oxygen vacancies played a crucial role in enhancing the catalytic performance and reaction kinetics.
JOURNAL OF CATALYSIS
(2021)
Article
Engineering, Environmental
Yanan Chong, Tingyu Chen, Yifei Li, Jiajin Lin, Wei-Hsiang Huang, Chi-Liang Chen, Xiaojing Jin, Mingli Fu, Yun Zhao, Guangxu Chen, Jiake Wei, Yongcai Qiu, Geoffrey I. N. Waterhouse, Daiqi Ye, Zhang Lin, Lin Guo
Summary: Enhancing oxygen activation through defect engineering is an effective strategy for boosting catalytic oxidation performance. The study demonstrates that quenching is an effective strategy for preparing defect-rich Pt/metal oxide catalysts with superior catalytic oxidation activity. The quenching process creates abundant lattice defects and lattice dislocations in the support, promoting stronger electronic interactions between Pt species and the support, leading to higher oxidation Pt species generation for modulating the adsorption/desorption behavior of reactants.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Hai-Chao Sun, Kun Yuan, Wang-De Hua, Zi-Rui Gao, Qian Zhang, Chen-Yue Yuan, Hai-Chao Liu, Ya-Wen Zhang
Summary: The metal-support interface plays a crucial role in heterogeneous catalysis by influencing catalytic efficiency. This study presents a strategy to optimize the interfacial activity of Co/ CeO2 catalysts for the water-gas shift reaction (WGSR) through a simple NH3 treatment process. The NH3 treatment weakens the metal-support interaction and induces oxygen vacancy generation, resulting in improved CO adsorption and activation ability. This combination of effects enhances the catalytic efficiency for the WGSR via the carboxyl pathway at low temperatures.
Article
Chemistry, Physical
Xiao-Chen Sun, Kun Yuan, Wang-De Hua, Zi-Rui Gao, Qian Zhang, Chen-Yue Yuan, Hai-Chao Liu, Ya-Wen Zhang
Summary: The metal-support interface is crucial in heterogeneous catalysis, and modulation of the metal-support interaction can enhance catalytic efficiency. In this study, a NH3 treatment process was used to modulate the interface interaction of Co/CeO2 catalysts for the water-gas shift reaction (WGSR). The treatment resulted in improved catalytic activity by weakening the metal-support interaction, enhancing CO adsorption and activation, and inducing oxygen vacancy generation. The active interface construction could be extended to other catalysts and has great potential in various chemical transformation reactions and industrial catalysis.
Article
Chemistry, Physical
Yanbo Deng, Shijie Liu, Lian Fu, Yi Yuan, Anmin Zhao, Dajun Wang, Heng Zheng, Like Ouyang, Shaojun Yuan
Summary: The efficiency of CO oxidation catalysts can be improved under wet conditions by controlling the metal-support interaction of Pd/Pr-CeO2 catalysts.
JOURNAL OF CATALYSIS
(2023)
Article
Biochemistry & Molecular Biology
Tiantian Zhang, Jiacheng Xu, Yan Sun, Shiyu Fang, Zuliang Wu, Erhao Gao, Jiali Zhu, Wei Wang, Shuiliang Yao, Jing Li
Summary: Pt-based catalysts exhibit unique catalytic properties, and the metal-support interactions play a crucial role in enhancing catalytic activity. This study investigated the interaction between 1 wt% Pt nanoparticles on beta-MnO2 support during carbon monoxide oxidation. The results showed that the presence of Pt inhibited CO oxidation below 210 degrees C but promoted it above 210 degrees C. The mechanism of Pt-beta-MnO2 interaction and its effect on CO oxidation were proposed based on the operando DRIFTS-MS results.
Article
Chemistry, Inorganic & Nuclear
Xianxian He, Hongfei Liu, Jiangzhou Qin, Zhaodong Niu, Jincheng Mu, Baojun Liu
Summary: The electrochemical reduction of nitrate (NO3-) to ammonia (NH3) has been successfully achieved using a heterostructured Co/Co3O4 electrocatalyst anchored on N-doped carbon nanotubes. The catalyst exhibits high selectivity and efficiency, with a faradaic efficiency of up to 67% and a yield of 8.319 mg h(-1) mg(cat)(-1). Additionally, it shows excellent long-term stability. Isotopic labelling experiments confirm that the produced NH3 originates from NO3- species. In situ electrochemical Raman spectra provide insights into the stable structure of the catalyst and identify possible intermediates during the electrocatalytic NO3- reduction reaction (NO3RR).
DALTON TRANSACTIONS
(2023)
Article
Engineering, Chemical
Qiuyu Shen, Zhihui Lu, Fukun Bi, Dongfeng Zhang, Lijuan Li, Xiaodong Zhang, Yiqiong Yang, Minghong Wu
Summary: In this paper, three different reduction methods were used to synthesize Pt-loaded Co3O4, and it was found that the catalyst produced by the NaBH4 reduction method had the best activity. Through characterization and experiments, it was revealed that this synthesis method optimized the electronic metal-support interaction (EMSI) of the catalyst, leading to electron transfer between Pt species and Co3O4. The catalysts also showed excellent water resistance, stability, and recycling performance, and the possible degradation mechanism of toluene was revealed as well.
SEPARATION AND PURIFICATION TECHNOLOGY
(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
Yuan Li, An Guo, Ying Yang, Guangyin Fan
Summary: Developed a stepwise activation strategy to produce highly active and reusable Rh/CoFe2O4-SB-H2 catalyst with abundant oxygen vacancies and strong electronic metal-support interaction. This catalyst showed excellent performance in hydrogen production from ammonia borane hydrolysis and oxygen generation from H2O2 decomposition under ultrasound irradiation. The strategies developed here can be applied to enhance the performance of other reducible metal oxides supported metal catalysts.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Yang Yang, Wenjian Fang, Yan Mi, Jiawei Yan, Xiaochuan Li, Wenfeng Shangguan
Summary: This paper presents a new method to introduce surface and bulk defects in SrTiO3 nanocrystals. The reducing agent, melamine, was carbonized under a nitrogen atmosphere to generate reductive NH3 and C, which reduced the SrTiO3 nanocrystals. The relative concentration ratio of bulk defects to surface defects in SrTiO3 nanocrystals could be tuned by this reduction treatment. The effects of surface and bulk defects on the band structures of SrTiO3 were studied, and it was found that the surface oxygen defects shifted the band structure to a higher energy level, while the bulk oxygen defects restored the energy levels of the band structure. Therefore, by adjusting the relative concentration ratio of bulk defects to surface defects in SrTiO3, the photocatalytic water splitting activity can be significantly improved.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Zhongyan Wang, Chengsheng Yang, Xianghong Li, Xiwen Song, Chunlei Pei, Zhi-Jian Zhao, Jinlong Gong
Summary: This study investigates the role of CO2 dissociation on the CoCu surface during the reaction and achieves different selectivity to ethanol by using different silica supports to tune the metal-support interaction.
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
Materials Science, Multidisciplinary
Yang Wang, Sai Chen, Jiachen Sun, Yufei Xie, Zhi-Jian Zhao, Chunlei Pei, Jinlong Gong
Summary: This paper investigates the roles of V-O sites on propane dehydrogenation (PDH) over supported monomeric VOx species. Results show that the V-O-S site plays a decisive role in PDH, while V-OH and V=O sites have minimal influence. Additionally, ZrO2 exhibits higher specific activity due to the discrepant Lewis acidity of different V-O-S sites.
SCIENCE CHINA-MATERIALS
(2023)
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
Nanoscience & Nanotechnology
Xin Chang, Zhi-Jian Zhao, Zhenpu Lu, Sai Chen, Ran Luo, Shenjun Zha, Lulu Li, Guodong Sun, Chunlei Pei, Jinlong Gong
Summary: In this study, a methodology was proposed to describe the microenvironment and determine the effectiveness of active sites in single-site alloys, using a simple descriptor called degree-of-isolation, which considers both electronic regulation and geometric modulation within a PtM ensemble. The catalytic performance of PtM single-site alloy for propane dehydrogenation was thoroughly examined, revealing a volcano-shaped isolation-selectivity plot that shows a Sabatier-type principle for designing selective single-site alloys.
NATURE NANOTECHNOLOGY
(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
Multidisciplinary Sciences
Wei Wang, Sai Chen, Chunlei Pei, Ran Luo, Jiachen Sun, Hongbo Song, Guodong Sun, Xianhui Wang, Zhi-Jian Zhao, Jinlong Gong
Summary: By coupling chemical looping-selective hydrogen combustion and multifunctional catalysts, we achieved high propylene selectivity in the direct propane dehydrogenation reaction. The reaction mechanism is influenced by the proximity between the dehydrogenation and combustion sites.
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, 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.
