Article
Chemistry, Physical
Hua Zhou, Hui-Qiong Wang, Jin-Cheng Zheng, Xiao-Dan Wang, Yufeng Zhang, Junyong Kang, Lihua Zhang, Kim Kisslinger, Rui Wu, Jia-Ou Wang, Hai-Jie Qian, Kurash Ibrahim
Summary: This study investigates the heteroepitaxial and energy band structures of STO/ZnO interfaces, showing different azimuth orientations and rotation domains of STO films on ZnO substrates. The downward band structures at the STO/ZnO interfaces were confirmed by experimental and theoretical methods, indicating an asymmetry between STO/ZnO and ZnO/STO interfaces.
APPLIED SURFACE SCIENCE
(2021)
Article
Materials Science, Multidisciplinary
Hua Zhou, Hui-Qiong Wang, Jin-Cheng Zheng, Xiao-Dan Wang, Yufeng Zhang, Junyong Kang, Lihua Zhang, Kim Kisslinger, Rui Wu, Jia-Ou Wang, Hai-Jie Qian, Kurash Ibrahim
Summary: The electronic structure of the STO/ZnO heterointerface was investigated using in situ photoemission spectroscopy and X-ray absorption spectroscopy, revealing the formation of polar interfaces and electron transfer phenomena.
RESULTS IN PHYSICS
(2021)
Article
Energy & Fuels
Hao Chen, Haishuai Cui, Yang Lv, Pingle Liu, Fang Hao, Wei Xiong, He'an Luo
Summary: Cu/ZnO/ZrO2 catalysts with different ZnO morphologies were prepared and used for CO2 hydrogenation to methanol. The catalyst with flower-like ZnO morphology showed the highest catalytic performance and possess the most oxygen vacancies. The experimental results and DFT calculations suggest that oxygen vacancies play a crucial role in promoting the reaction and reducing the energy barriers.
Article
Chemistry, Physical
Won Hui Doh, Hiroshi Kondoh, Eonhyoung Ahn, Dohyun Park, Daeheum Cho, Chang Min Kim
Summary: The interaction between ethene and Cl-2 on ZnO(000 (1) over bar) was studied using X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption (TPD), and density functional theory (DFT) calculations. Cl-2 was found to adsorb perpendicularly on ZnO(000 (1) over bar) at 110 K and dissociate on the surface at 200-230 K. When the surface was coadsorbed with Cl-2 and ethene, the desorption of 1,2-dichloroethane was observed at around 230 K, indicating the direct chlorination of C2H4 by hot Cl atoms produced during Cl-2 dissociation.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Applied
Jing Wang, Kaihang Sun, Xinyu Jia, Chang-jun Liu
Summary: Highly dispersed Rh/In2O3 catalyst prepared by deposition-precipitation method shows excellent activity and selectivity for CO2 hydrogenation to methanol, promoting the reaction even at lower temperatures.
Article
Chemistry, Physical
Ang Cao, Zhenbin Wang, Hao Li, Jens K. Norskov
Summary: The study investigated the catalytic activity of In2O3 (111) and In2O3 (110) in methanol synthesis, finding a relationship between the number of reduced surface In layers and catalytic activity. By adding a ZrO2 support, the activity of In2O3 catalyst in methanol formation can be optimized.
Article
Energy & Fuels
Rajan Singh, Komal Tripathi, Kamal Kishore Pant
Summary: The study focuses on CeO2, ZrO2 and ZnO supported Cu catalysts, with Cu/ZnO showing the highest CO2 conversion rate and Cu/CeO2 demonstrating over 90% methanol selectivity at lower temperatures. The high methanol selectivity of Cu/CeO2 catalyst may be attributed to its excess surface oxygen vacancies and higher basic site density.
Article
Energy & Fuels
Ziqi Li, Tao Du, Yingnan Li, He Jia, Yisong Wang, Yanli Song, Xin Fang
Summary: In this study, oxygen vacancy rich Cu-ZnO-ZrO2 catalysts were prepared via a facile solid-state method. These catalysts exhibited remarkable performance in CO2 hydrogenation reactions with high methanol selectivity. The preparation process is simple, without wastewater generation, and no reduction is required. The oxygen vacancies in these catalysts benefit the adsorption of CO2 and the migration of intermediates, enhancing methanol formation and selectivity.
Article
Engineering, Environmental
Mingming Luo, Jiayao Li, Meiling Wang, Yongqing Ma, Ganhong Zheng, Min Wang, Yitong Zhou
Summary: By optimizing the surface-active sites, we reported the electrocatalytic conversion of CH4 into CH3COOH in HCO3--contained electrolyte. A high CH3COOH yield of 347.31 mmol gcat-1 h-1 and a CH3COOH selectivity of 85.4% were obtained over the optimal catalyst. This CH3COOH yield is 2-5 orders of magnitude higher than previous reports. Our work provides new insight into the design of highly active and selective catalysts for CH4 electrocatalytic conversion into CH3COOH.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Physical
Ersen Mete, Sinasi Ellialtioglu, Oguz Gulseren, Deniz Uner
Summary: In this study, the concentration and coordination of surface oxygen vacancies were found to be critical for the direct water-splitting reaction on PbTiO3 and TiO2 (001) surfaces. Two neighboring O vacancies are necessary for water-splitting on TiO2-terminated surfaces, while only two oxygen vacancies are required for molecular hydrogen formation on the PbO-terminated surface of PbTiO3. However, the formation of molecular hydrogen is hindered by the presence of a third vacancy on TiO2-terminated surfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Review
Materials Science, Ceramics
Vitaly Gurylev, Tsong Pyng Perng
Summary: Defects in zinc oxide (ZnO) play a crucial role in influencing its properties and applications, with potential for improved characteristics through the introduction of oxygen and zinc vacancies. Defective ZnO shows broad application potential in nanoscale devices, yet faces challenges and requires further research for in-depth exploration.
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
(2021)
Article
Engineering, Environmental
Xilong Wang, Mohnnad H. Alabsi, Xingzhu Chen, Aijun Duan, Chunming Xu, Kuo-Wei Huang
Summary: PdZn/CTD catalysts with CeTi bimetallic modified dendritic mesoporous silica nanospheres as supports exhibit excellent catalytic performance for CO2 hydrogenation to methanol. The optimized catalysts demonstrate high methanol yield, selectivity, and stability, and the reaction mechanism is found to involve HCOO* and CH3O* intermediates.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Chaojie Huang, Zhaoxuan Wu, Hu Luo, Shunan Zhang, Zilong Shao, Hui Wang, Yuhan Sun
Summary: The study successfully improved the performance of CO2 hydrogenation at high temperature using a Pd/ZnZr catalyst, achieving high methanol selectivity and yield.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Applied
Chenyang Shen, Qianqian Bao, Wenjuan Xue, Kaihang Sun, Zhitao Zhang, Xinyu Jia, Donghai Mei, Chang-jun Liu
Summary: Nickel catalyst supported by indium oxide has been proven to be highly active for CO2 hydrogenation to methanol, with the RWGS pathway being the most theoretically favored. It has been demonstrated that the interfacial oxygen vacancy serves as an active site for promoting CO2 hydrogenation by facilitating charge transfer between nickel species and indium oxide.
JOURNAL OF ENERGY CHEMISTRY
(2022)
Article
Chemistry, Physical
Xuelian Chen, Xiang Li, Qihua Yang, Can Li
Summary: This study demonstrates that the activity of ZnZrOx catalyst in steam reforming of methanol (SRM) at low temperatures can be greatly enhanced by doping a small amount of copper. The introduction of copper in CuZnZrOx ternary solid solutions rich in oxygen vacancies leads to efficient water activation and faster generation and decomposition of the HCOOH intermediate. The coexistence of low-valence copper and oxygen vacancies contributes to the excellent performance of CuZnZrOx in SRM.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Jing Liu, Christof Haettig, Sebastian Hoefener
JOURNAL OF CHEMICAL PHYSICS
(2020)
Article
Chemistry, Multidisciplinary
Bin Hu, Lisa Warczinski, Xiaoyu Li, Mohong Lu, Johannes Bitzer, Markus Heidelmann, Till Eckhard, Qi Fu, Jonas Schulwitz, Mariia Merko, Mingshi Li, Wolfgang Kleist, Christof Hattig, Martin Muhler, Baoxiang Peng
Summary: This study demonstrates an efficient method for the hydrogenolysis of HMF to DMF under mild reaction conditions using Pd nanoparticles supported on N-containing and N-free mesoporous carbon materials, along with formic acid (FA) and hydrogen. It was found that the main role of FA is to shift the dominant reaction pathway from the hydrogenation of the aldehyde group to the hydrogenolysis of the hydroxymethyl group, thereby significantly enhancing the reaction rate. The interaction between Pd2+ species and pyridine-like N atoms was shown to enhance the selective hydrogenolysis of the C-OH bond in the presence of FA, leading to the stabilization of H-.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
S. Ghidinelli, G. Longhi, S. Abbate, C. Haettig, S. Coriani
Summary: UV-vis absorption and magnetic circular dichroism spectra of naphthalene and its derivatives were simulated using CC2 and TD-DFT methods. CC2 simulations showed the best agreement with experimental data. Analysis of electric dipole and magnetic dipole transition moments helped interpret electronic transitions and Faraday B term inversion among naphthalene derivatives.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Physical
Daniil A. Fedotov, Sonia Coriani, Christof Haettig
Summary: The study presents an implementation of a complex solver for computing the complex response functions of damped response theory. The solver uses a partitioned formulation to avoid storing double excitation amplitudes, making it widely applicable in the context of the resolution-of-identity (RI) coupled cluster singles and approximate doubles (CC2) method.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Lisa Warczinski, Christof Haettig
Summary: The study using density functional theory (DFT) discusses the process of hydrogen spillover on metal nanoparticle decorated carbon surfaces, showing that graphitic nitrogen atoms and water molecules play significant roles in facilitating the hydrogen spillover reaction.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Arjeta Rushiti, Christof Haettig, Bo Wen, Annabella Selloni
Summary: Research suggests that CFO may be a promising oxidation catalyst due to its relatively low energy cost of vacancy formation and strong affinity towards water, making it more competitive than NiCo2O4 and Co3O4.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Shota Tsuru, Bikramjit Sharma, Masanari Nagasaka, Christof Haettig
Summary: Solvent-solute electrostatic interactions and solvent configuration fluctuations can affect solute excitation energies, potentially dominating dynamics in solution systems and causing shifts or broadening of absorption peaks. Experimental absorption spectra of a solute in aqueous solution were accurately reproduced by combining theoretical treatment of explicit local solvation structures with the COSMO solvation model for long-range solvation.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Arjeta Rushiti, Christof Haettig
Summary: This study investigated the pathways of dioxygen activation on the (001) surfaces of cobalt ferrite using density functional theory. The results suggest that activation is promoted by electron transfer from d metal centers onto the adsorbed oxygen, with subsequent dissociation of dioxygen and surface reoxidation identified as critical steps that may limit the rate of the oxidation processes.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Robert S. Tress, Christof Haettig, Sebastian Hoefener
Summary: In this work, a modified frozen density embedding method is proposed to reduce charge spill-out and improve the consistency of calculations by adding all-electron pseudopotentials.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Multidisciplinary
Niklas Suelzner, Julia Haberhauer, Christof Haettig, Arnim Hellweg
Summary: In this contribution, the conductor-like screening model for realistic solvation (COSMO-RS) is extended to predict pK(a) values in acetone. 120 organic acids were analyzed using COSMO-RS, and the results showed that the data set can be divided into two groups, with the phenols being different from the other three subsets. The acrylic and benzoic acids and the sulfonamides can be treated together and yield an excellent linear correlation, while the phenols exhibit a slope larger than one.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Robert S. Tress, Jing Liu, Christof Haettig, Sebastian Hoefener
Summary: Frozen density embedding (FDE) is a simple and user-friendly embedding method for complex environments. Combining FDE with pair natural orbitals (PNOs) reduces computation time. Tests on TAPP molecular crystals show that the truncation error of PNO-based wavefunction methods is smaller than the shifts themselves, allowing for a combination with the FDE method.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Niklas Suelzner, Christof Haettig
Summary: This study applies the thermodynamic Förster cycle to investigate the excited-state pKa values of pyranine-derived superphotoacids. The results show that the calculated electronic excitations agree well with experimental data, suggesting the validity of this approach. The calculations also reveal that the redistribution of charge from the hydroxy group to the aromatic ring and electron-withdrawing substituents is the origin of photoacidity for these superphotoacids.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Physical
Shota Tsuru, Bikramjit Sharma, Dominik Marx, Christof Haettig
Summary: This study investigates the impact of sampling methods on spectral broadening in the gas phase and on the convergence of spectra in aqueous solution using microsolvation, continuum solvation, and hybrid models with pyrazine as a test case. The results show that static and time-resolved X-ray absorption spectra obtained with Wigner and Maxwell-Boltzmann samplings in the gas phase agree well. In aqueous solution, only the first two energetically low-lying bands converge quickly with the size of the explicitly included solvation shells, indicating the importance of continuum solvation in computational UV-vis absorption spectra.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Arjeta Rushiti, Tobias Falk, Martin Muhler, Christof Haettig
Summary: By using density functional theory and an embedded cluster model, we investigated the surface structure and reactivity of cobalt ferrite, finding that adsorbates exhibit different behaviors depending on the adsorption sites.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Sarah Karbalaei Khani, Bastian Geissler, Elric Engelage, Patrick Nuernberger, Christof Haettig
Summary: By investigating the absorption and fluorescence of halogenated imidazolium compounds in acetonitrile solution with different counterions and their ability as halogen-bond donors, spectroscopic signatures and photoinduced dynamics associated with ion-pairing were identified through experimental measurements and quantum chemical calculations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)