Article
Multidisciplinary Sciences
Pushkar G. Ghanekar, Siddharth Deshpande, Jeffrey Greeley
Summary: This paper presents a catalyst surface model called ACE-GCN, which takes into account various atomic configurations and successfully describes the influence of atomic-scale factors in heterogeneous catalytic reactions. The use of this model accelerates the development of rigorous descriptions of catalyst surfaces under in-situ conditions.
NATURE COMMUNICATIONS
(2022)
Article
Multidisciplinary Sciences
Jiwon Kim, Jae Hyung Kim, Cheoulwoo Oh, Hyewon Yun, Eunchong Lee, Hyung-Suk Oh, Jong Hyeok Park, Yun Jeong Hwang
Summary: An electro-assisted approach using acid-treated carbon electrocatalyst and in-situ cathodically generated reactive oxygen species is proposed for the partial oxidation of methane at ambient temperature and pressure. Reactive oxygen species activate methane and methanol, leading to selective methane partial oxidation. This study presents a method for the electrochemically assisted partial oxidation of methane to produce liquid oxygenate, HCOOH, selectively.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Feng Yi, Shane Q. Arlington, Justin Gorham, William Osborn, Ethan J. Crumlin, Slavomir Nemsak, David A. LaVan
Summary: The formation and thermal stability of Pt surface oxides on a Pt thin film were studied using ambient-pressure X-ray photoelectron spectroscopy. The results showed that at a certain oxygen pressure, the Pt surface oxide was formed and decomposed during heating and cooling processes, which is important for understanding the surface states and catalytic mechanisms of platinum films.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Environmental Sciences
Tiancheng Wen, Jing Wang, Jian Zhang, Chao Long
Summary: In this study, α-MnO2 nanorods with tunable oxygen vacancies and hydroxyl groups were synthesized to enhance the deep oxidation of toluene. The as-synthesized nanorods showed superior activity and high COx selectivity, promoting the deep oxidation of toluene. It was found that the increase of oxygen vacancies and hydroxyl groups concentration contributed to the enhancement of performance.
ENVIRONMENTAL RESEARCH
(2023)
Article
Energy & Fuels
Xuexia Zhang, Lei Huang, Yu Jiang, Long Lin, Hongbo Liao, Wentao Liu
Summary: This paper presents a comprehensive analysis of the polarization processes during accelerated performance degradation in fuel cells. The study reveals that the growth of platinum oxides plays a dominant role in the accelerated decline of performance, leading to early decay at low current density and sudden concentration polarization at high current density. The formation and reduction of platinum oxide also affect voltage stability and the steady performance of loading and unloading processes.
Article
Multidisciplinary Sciences
Jialun Gu, Lanxi Li, Youneng Xie, Bo Chen, Fubo Tian, Yanju Wang, Jing Zhong, Junda Shen, Jian Lu
Summary: This study presents a Turing structuring strategy that utilizes high-density nanotwins to activate and stabilize ultra-thin metal nanosheets as efficient electrocatalysts for hydrogen evolution reaction. The Turing PtNiNb nanocatalyst exhibits significantly improved mass activity and stability compared to commercial Pt/C, and the stability is also demonstrated in an anion-exchange-membrane water electrolyser.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Xiaoran Niu, Ru-Yang Shao, Le Zhang, Cong Xu, Tian-Wei Song, Peng Yin, Lei Tong, Chenliang Su, Hai-Wei Liang
Summary: We investigated the effects of wet-impregnation and oleylamine-mediated colloid methods on the synthesis of PtCo intermetallic catalysts on different porous carbon supports. It was found that efficient utilization of the internal surface area of porous carbon supports is crucial for the synthesis of small-sized PtCo intermetallic catalysts, which is highly dependent on the metal deposition method and the pore structure of the carbon supports. As a result, small-sized PtCo intermetallic catalysts with enhanced oxygen reduction reaction activity and improved proton exchange membrane fuel cell performance were prepared using the wet-impregnation method on mesoporous carbon supports.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Physical
Bangfen Wang, Xiufeng Li, Yuhai Sun, Hailin Xiao, Mingli Fu, Shuhua Li, Hong Liang, Zhiwei Qiao, Daiqi Ye
Summary: Pt/CeO2 catalysts were modified with non-thermal plasma to enhance the catalytic activity for toluene oxidation. The plasma treatment affected the Pt particle size, CeO2-rod length, oxygen vacancy concentration, and Pt/CeO2 reducibility. The impact of plasma on Pt atoms was more significant than on oxygen vacancies.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Engineering, Environmental
Minghui Cui, Feilong Wang, Wenqi Zhao, Dai Zhang, Rongqing Liang, Qiongrong Ou, Shuyu Zhang
Summary: Green hydrogen is produced by electrolyzing water using renewable energy, thereby generating hydrogen with zero carbon emissions. Platinum-based catalysts are highly efficient, but limited by their high price and low availability. Researchers have synthesized a catalyst combining platinum single atoms and nanoparticles using nonthermal plasma technique, which exhibits excellent performance at high current density and a significantly lower loading compared to commercial catalysts. This technique offers a low-cost and efficient method to synthesize high-current hydrogen evolution reaction catalysts, promoting their industrial development.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Jan Kloppenburg, Livia B. Partay, Hannes Jonsson, Miguel A. Caro
Summary: A Gaussian approximation machine learning interatomic potential for platinum is developed based on density-functional theory (DFT) data. The potential exhibits excellent transferability and agreement with DFT in various properties such as bulk elasticity, surface energetics, and nanoparticle stability. It provides state-of-the-art accuracy at a low computational cost. Two examples are presented to demonstrate the potential's capability in modeling Pt systems: the pressure-temperature phase diagram of Pt calculated using nested sampling and a study of the spontaneous crystallization of a large Pt nanoparticle based on classical dynamics simulations over several nanoseconds.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Review
Chemistry, Multidisciplinary
Max J. Hulsey, Sikai Wang, Bin Zhang, Shipeng Ding, Ning Yan
Summary: Single-atom catalysts offer unique advantages but are often intrinsically ill-defined. In this Account, we describe approaches to break down the complexity of supported single-atom catalysts through the careful choice of oxide supports with specific binding motives as well as the adsorption of well-defined ligands. We utilized polyoxometalate-supported single-atom catalysts as ideal systems for the in situ spectroscopic study of single atom sites during reactions.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Multidisciplinary Sciences
Lingyou Zeng, Zhonglong Zhao, Fan Lv, Zhonghong Xia, Shi-Yu Lu, Jiong Li, Kaian Sun, Kai Wang, Yingjun Sun, Qizheng Huang, Yan Chen, Qinghua Zhang, Lin Gu, Gang Lu, Shaojun Guo
Summary: In water splitting electrolyzers, platinum single-atom catalysts show remarkable catalytic activity and stability for anodic oxygen evolution. Their superior performance is attributed to the unique coordination with cobalt hydrogen phosphate and the suppression of soluble platinum species. Utilizing alkaline water electrolyzers with ultra-low platinum loading achieves industrial-level current density and high durability.
NATURE COMMUNICATIONS
(2022)
Article
Physics, Fluids & Plasmas
Pierre Naze
Summary: The objective of this work is to demonstrate the similarities between adiabatic and isothermal processes. By examining the criteria for the compatibility of linear-response theory with the second law of thermodynamics in thermally isolated systems, we find that they are the same as those for isothermal processes. This leads us to explore the thermodynamic consequences of time-average excess work, demonstrating the existence of a well-defined relaxation time obeying the second law of thermodynamics in thermally isolated systems. We apply this understanding to the Landau-Zener model, observing negative entropy production rates for nonmonotonic and rapid protocols.
Article
Multidisciplinary Sciences
Yong Wang, Pengju Ren, Jingting Hu, Yunchuan Tu, Zhongmiao Gong, Yi Cui, Yanping Zheng, Mingshu Chen, Wujun Zhang, Chao Ma, Liang Yu, Fan Yang, Ye Wang, Xinhe Bao, Dehui Deng
Summary: A unique structure design of Pt isolated by graphene was reported for efficient catalytic CO oxidation in an oxygen-rich atmosphere, achieving nearly 100% CO conversion at room temperature. This catalyst showed distinct behavior from classical metal-metal oxide interfaces and provided a new direction for the design of heterogeneous catalysts.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Lixin Su, Junxiang Chen, Fulin Yang, Peng Li, Yiming Jin, Wei Luo, Shengli Chen
Summary: The kinetic pH effect in hydrogen electrocatalysis, particularly the difference in kinetics between hydrogen oxidation and evolution reactions in acidic and alkaline electrolytes, remains controversial. Evaluating the kinetics of these reactions on precious metal-based electrocatalysts across a wide pH range, we discover a universal inflection-point behavior, where the inflection point pH and the acid-alkaline activity gap depend on the catalyst's hydroxide binding energy. Our results suggest that the formation of adsorbed hydroxide improves the hydrogen-bond network in the electric double layer, thus promoting the kinetics of hydrogen oxidation and evolution.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Erhao Gao, Wenjing Feng, Qi Jin, Li Han, Yi He
Summary: The influence of K-doping on the reactive oxygen species and elementary reactions of HCHO catalytic oxidation was investigated using density functional theory (DFT). The introduction of K-doping changed the electronic structures of Ce and O, facilitating the adsorption and activation of HCHO and O2 molecules, enhancing lattice oxygen mobility, and reducing the energy barrier for HCHO oxidation. K-doping also promoted the formation of hydroxyl groups, facilitating HCHO adsorption and oxidation.
Article
Chemistry, Physical
Hao Fu, Zhangliang Xu
Summary: In this study, the adsorption mechanisms and detection performance of formaldehyde, ammonia, and sulfur dioxide on undoped and metal-doped ZnO surfaces were investigated using density functional theory. The results showed that formaldehyde and ammonia were physically adsorbed on the undoped ZnO surface, while sulfur dioxide was weakly chemisorbed. The adsorption energy was enhanced when ZnO was doped with metals. These findings provide theoretical guidance for the application of ZnO substrate materials in gas sensitivity research.
Article
Chemistry, Physical
Atsushi Nomura, Tohru Kurosawa, Migaku Oda, Satoshi Demura, Shogo Kuwahara, Sora Kobayashi, Hideaki Sakata
Summary: The study investigates the tunneling spectra of 1T-TiSe2 in the CDW state and the dip structure below the Fermi level, aiming to determine whether this dip is a CDW gap. The answer to this question is crucial for understanding the driving mechanism of CDW.
Article
Chemistry, Physical
A. S. Petrov, D. I. Rogilo, A. I. Vergules, V. G. Mansurov, D. V. Sheglov, A. V. Latyshev
Summary: This study investigates Si mass transport and morphological transformations on the Si(111) surface during (root 3 x root 3)-Sn reconstruction formation and Si homoepitaxy. The research shows that the formation of different Sn phases at different temperatures affects the Si island nucleation and monatomic step shift, which in turn impact the morphology of the Sn/Si(111) interface. Electromigration-induced drift of disordered Sn domains leads to enhanced noncompensated Si mass transport and surface roughening.
Article
Chemistry, Physical
D. V. Gruznev, L. V. Bondarenko, A. Y. Tupchaya, A. A. Yakovlev, A. N. Mihalyuk, A. V. Zotov, A. A. Saranin
Summary: Deposition of thallium (Tl) onto the Au/Si(111)5 x 2 reconstruction followed by annealing results in the formation of a surface structure with 4 x 2 periodicity. The immiscibility of Au and Tl leads to the migration of Tl atoms over the Si chains. Thallium donates electrons to the surface, converting the metallic surface into an insulating state and altering the inter-chain distance within the array of Au atomic wires.
Article
Chemistry, Physical
Simone Giusepponi, Francesco Buonocore, Barbara Ferrucci, Massimo Celino
Summary: Using ab-initio calculations, the interaction between lead adatom and both clean and doped iron (100) surfaces was investigated. It was found that the lead adatom prefers to adsorb in the hollow site, which is more stable compared to the top and bridge sites, and in this position, it is energetically favorable over the iron adatom. Moreover, lead adsorbed in the hollow site of the iron (100) surface doped with chromium was found to create a more stable system compared to nickel-doped surfaces with an iron adatom in the same position. The study also explored inter-layer distances, bonding mechanisms, magnetic behaviors, and charge density differences. The results provide insights into the role of doping in the interaction between lead adatom and iron surface, and have implications for the analysis of corrosion processes caused by liquid lead.
Article
Chemistry, Physical
Shuo Zhang, Jin-Ho Choi
Summary: The recent synthesis of two-dimensional layered WSi2N4 has attracted attention due to its potential applications. This study investigates the catalytic performance of WSi2N4 monolayers with nitrogen vacancies in the hydrogen evolution reaction using first-principles calculations. The results show that the defective WSi2N4 monolayers exhibit remarkably high catalytic activity comparable to platinum catalysts. Electronic structure calculations also reveal the emergence of spin-polarized states due to the introduction of nitrogen vacancies.
Article
Chemistry, Physical
Xiaoyan Yu, Xin Cao, Wei Kang, Shanhua Chen, Ao Jiang, Yuhao Luo, Wenwei Deng
Summary: First-principles calculations were used to investigate the electronic properties of a TiO2 heterostructure modified with Bi2Te3 co-catalyst. The study revealed that the Bi2Te3/TiO2 interface introduced optimal band offsets, effectively suppressing electron-hole recombination and enhancing the utilization efficiency of photo-generated carriers. Additionally, the Bi2Te3 co-catalyst introduced extra catalytic active sites, further boosting the photo-catalytic hydrogen evolution efficiency.
Article
Chemistry, Physical
Filippo Longo, Emanuel Billeter, Selim Kazaz, Alessia Cesarini, Marin Nikolic, Aarati Chacko, Patrik Schmutz, Zbynek Novotny, Andreas Borgschulte
Summary: Alkaline water electrolysis is a simple and efficient method for renewable hydrogen production, utilizing cheap and abundant transition metals. The catalytic properties of Ni materials are enhanced by the formation of oxidized compounds on the surface. The high electrocatalytic activity of Ni (oxy)-hydroxides is directly related to water intercalation in the passivation layer, supporting the hypothesis of a water mediated OH- diffusion mechanism. The self-organization of the surface structure during passivation layer formation enables high electrode performance.
Article
Chemistry, Physical
Mohan Kumar Kuntumalla, Miriam Fischer, Alon Hoffman
Summary: By investigating the bonding, retention, and thermal stability of nitrogen in H-Diamond (100), it was found that nitrogen can partially recover its bonding with carbon atoms after high-temperature annealing, indicating a high thermal stability of nitrogen in diamond.
Article
Chemistry, Physical
Dong Yue, Liangying Wen, Rong Chen, Jianxin Wang, Zhongqing Yang
Summary: The adsorption behavior of Cl2 molecules on the TiC surface and the formation and transfer of reaction products were studied using first-principles ab initio calculations. The results show that the Cl atoms bonded to the surface Ti atoms are more stable, and the TiCl3 intermediate is easier to form than the TiCl2 intermediate.
Article
Chemistry, Physical
Yatao Wang, Peng Zhang, Hongjuan Li, Qiuju Xu, Shujun Liu, Xiaopeng Liu, Xuehua Guo, Yitao Li, Jinzhang Liu, Sen Dong, Zhi Wei Seh, Qianfan Zhang
Summary: In this study, the adsorption performance of two types of metal-organic frameworks (MOFs) for thiophene and benzene was experimentally investigated. The results showed that IZE-1 exhibited high selectivity and superior adsorption capacity for thiophene, especially at low concentrations. First-principles calculations and molecular dynamics simulations provided insights into the mechanism of thiophene adsorption and the high selectivity observed. This research demonstrates the potential of MOFs for thiophene adsorption, particularly at high concentrations.