Article
Environmental Sciences
Narcisse Tsona Tchinda, Lin Du, Ling Liu, Xiuhui Zhang
Summary: Using quantum chemical calculations and a cluster dynamics model, the role of pyruvic acid (PA) in the formation of sulfuric acid (SA) and aerosol particles was investigated. It was found that PA can potentially compete with water-catalyzed reaction in SA production and enhance particle formation in dry and polluted areas. The inclusion of this mechanism in aerosol models may reduce uncertainties in modeling the aerosol impact on climate.
ATMOSPHERIC CHEMISTRY AND PHYSICS
(2022)
Article
Multidisciplinary Sciences
Hongxia Hao, Itai Leven, Teresa Head-Gordon
Summary: Reaction rates of common organic reactions can significantly increase by several orders of magnitude in aqueous microdroplets compared to bulk solution. However, the reasons for this rate acceleration are still poorly understood. By studying the electric field distributions at the air-water interface, it has been found that the electric field alignments along free O-H bonds at the surface are on average around 16 MV/cm larger than those in the interior of the water droplet. This difference in electric field distribution may contribute to the enhanced surface reactivity observed in microdroplets.
NATURE COMMUNICATIONS
(2022)
Article
Multidisciplinary Sciences
Manuel F. Ruiz-Lopez, Marilia T. C. Martins-Costa, Joseph S. Francisco, Josep M. Anglada
Summary: Experimental and theoretical works have shown that the photochemistry of hydrogen peroxide (H2O2) at heterogeneous interfaces can be significantly influenced by surface properties. This finding opens up new perspectives for technological and biomedical applications.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Multidisciplinary
V. Manikandan, G. Ayyannan, Iulian Petrila, Rajaram S. Mane, Kamil Sobczak, J. Chandrasekaran, Robert D. Crapnell, Craig E. Banks
Summary: Ni-doped alumina nanoflakes show efficient and fast response to target gas SO3 at different concentrations, with improved response and shorter response time at higher temperatures. The sensor demonstrates stability and reproducibility over a long period of testing, making it suitable for practical applications. The Ni-dopant enhances oxygen adsorption and active sites, contributing to the excellent sensing properties.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Engineering, Environmental
Shideng Yuan, Xueyu Wang, Zhaoli Jiang, Heng Zhang, Shiling Yuan
Summary: This study used molecular dynamics simulations to investigate the role of nanobubbles in removing PFAS in aqueous environments. The results showed that the free energies of the air-water interface were lower than that of the bulk water region, indicating that the transformation of PFAS into the air-water interface is thermodynamically favorable. On the three-phase interface, PFBS can both move along the interface region and leave the interface region into the water phase, while PFOS tends to move along the interface region until it is captured by activated carbon.
Article
Chemistry, Multidisciplinary
Miguel de la Puente, Rolf David, Axel Gomez, Damien Laage
Summary: The acidity at the air-water interface decreases compared to the bulk, but is higher below the interface. This has important implications for environmental and biochemical processes.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Rahul Gera, Huib J. Bakker, Ricardo Franklin-Mergarejo, Uriel N. Morzan, Gabriele Falciani, Luca Bergamasco, Jan Versluis, Indraneel Sen, Silvia Dante, Eliodoro Chiavazzo, Ali A. Hassanali
Summary: This study investigates the properties of the water and surfactant C12E6 interface, finding that the addition of C12E6 near the critical micelle concentration enhances hydrogen bond strength and alters the orientation of water molecules. This leads to the formation of a broad interface with a large electric field, potentially opening up new possibilities for designing catalytic and light-harvesting systems at the water-surfactant-air interface.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Applied
Haobo Jin, Yongguo Jin, Jiajing Pan, Yi Sun, Long Sheng
Summary: This study investigated the structural transitions and molecular properties of ovalbumin, the most abundant protein in eggs, at the air-water interface using spectroscopic and molecular dynamics simulation techniques. The results showed that the alkaline environment and the air-water interface promoted the stretching of ovalbumin and increased its polarity, particularly for tryptophan. Electrostatic repulsion due to negative surface charges played a crucial role in the unfolding of ovalbumin. The study also found that non-hydrogen bonding forces were essential for protein migration.
FOOD HYDROCOLLOIDS
(2022)
Article
Biochemistry & Molecular Biology
Chengfeng Zhang, Lulu Cao, Yongkang Jiang, Zhiyao Huang, Guokui Liu, Yaoyao Wei, Qiying Xia
Summary: Through molecular dynamics simulations, this study investigates the interfacial adsorption, structures, and properties of n-dodecyl betaine (NDB) at the air-water interface at different surface coverages. The behavior of water molecules around the polar heads, the tilt angle of NDB molecules, and the length and conformation of the tail chain are analyzed. The study finds that surface coverage has little effect on the location and distribution of water molecules around the polar heads. As more NDB molecules are adsorbed, the number of hydrogen bonds between polar heads and water molecules slightly decreases, while their lifetimes increase.
Article
Chemistry, Physical
Xiaoqing Yu, Kuo-Yang Chiang, Chun-Chieh Yu, Mischa Bonn, Yuki Nagata
Summary: Insights into the microscopic structure of aqueous interfaces are important for understanding various processes on the water surface. The researchers used HD-SFG spectroscopy to probe these interfaces and showed the importance of correcting the measured spectra for local electromagnetic field effects. They compared different models to obtain an accurate representation of the interfacial water response and found that the Lorentz model provides a straightforward method for obtaining the molecular response in the hydrogen-bonded region.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Engineering, Environmental
Mingshan Zhang, Wenhui Li, Zhehui Jin
Summary: Molecular dynamic simulations reveal that deprotonated cyclohexanoic acid and heptanoic acid exhibit different interaction modes with water in pristine and hydroxylated carbon nanopores, which play a crucial role in the removal of NAs by activated carbons.
JOURNAL OF HAZARDOUS MATERIALS
(2021)
Article
Multidisciplinary Sciences
Xiangrui Kong, Dimitri Castarede, Erik S. Thomson, Anthony Boucly, Luca Artiglia, Markus Ammann, Ivan Gladich, Jan B. C. Pettersson
Summary: A surface-promoted sulfate-reducing ammonium oxidation reaction was found to occur spontaneously on common inorganic aerosol surfaces undergoing solvation, involving key intermediate species and leading to unexpected products. The discovery sheds light on chemistry uniquely associated with a solvating surface, presenting great potential to address current puzzles in heterogeneous chemistry.
Article
Chemistry, Physical
Tadini Wenyika Masaya, Fabien Goulay
Summary: The partitioning of small saccharide and amide molecules in aqueous droplets was studied using molecular dynamics. Organic molecules were modeled at the air-particle interface and surrounded by gaseous OH radicals. Results showed that molecules with polar functional groups were found predominantly in the water bulk, while molecules with alkyl groups migrated towards the interface. The simulations provided quantitative information about the air-water interface and the interaction between organic solutes and OH radicals, which is important in understanding oxidation mechanisms and kinetics within interfaces.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Yanqing Yang, Xiaoyu Sun, Mohammad Reza Poopari, Cuiying Jian, Hongbo Zeng, Tian Tang, Yunjie Xu
Summary: Chirality discrimination between R- or S-Tol-BINAP molecules and water-soluble serine chiral specie at a binary toluene/water interface is investigated for the first time using experimental interfacial tension measurements and molecular dynamic simulations. The results show that interfacial tension measurements can capture the preferential interactions between different pairs of enantiomers at liquid-liquid interfaces, providing a new approach for probing chirality discrimination.
Article
Chemistry, Physical
Tadini Wenyika Masaya, Fabien Goulay
Summary: The study employed molecular dynamics to investigate the distribution of saccharide and amide molecules between the surface and bulk of aqueous droplets. The simulations revealed that molecules with only polar functional groups tend to stay in the water bulk, while molecules with an alkyl group migrate towards the interface. Surface-active solutes near the water surface adopt a preferred orientation with the alkyl group facing the surface. The different packing arrangements in the interface influence solvation shell structures and the interaction between the organic molecules and absorbed OH radicals.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
David Deibert, Navneet Singh Khetrapal, Xiao Cheng Zeng
Summary: Large-sized gold anion clusters exhibit unique structural characteristics compared to other coinage metals. A 13-atom icosahedral core is typically formed in coinage metal nanoclusters at a cluster size of 55, whereas gold clusters do not acquire this core until the size reaches 60. This study investigates the robustness of the icosahedral core in large-sized gold anion clusters, revealing that the core persists in clusters with sizes ranging from 61 to 66. The shells of these clusters undergo significant structural deformations and polygonal defects to accommodate the exceptional stability of the core.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Songhua Cai, Jun Dai, Zhipeng Shao, Mathias Uller Rothmann, Yinglu Jia, Caiyun Gao, Mingwei Hao, Shuping Pang, Peng Wang, Shu Ping Lau, Kai Zhu, Joseph J. Berry, Laura M. Herz, Xiao Cheng Zeng, Yuanyuan Zhou
Summary: This study resolves the atomic-scale structural information on three prototypical intragrain interfaces using scanning transmission electron microscopy and establishes models for the calculation of electronic properties. The results show that these intragrain interfaces are generally electronically benign, but their interaction with point defects can have detrimental effects. This research contributes to a better understanding of the microscopic structure-property-performance relationship in metal halide perovskites.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Xiwen Zhang, Yilv Guo, Zhaobo Zhou, Xiuyun Zhang, Yunfei Chen, Xiao Cheng Zeng, Jinlan Wang
Summary: This study reports on the design of two new vdW magnetic multilayers with perfect spin-filtering capability and giant spin-filter energy-dependent tunnel magnetoresistance. These materials can be used as promising candidates for spin-based vdW devices and atomically thin magnetic information storage.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Bo Zhang, Shuo Sun, Yinglu Jia, Jun Dai, Dhanusha T. N. Rathnayake, Xi Huang, Jade Casasent, Gopi Adhikari, Temban Acha Billy, Yongfeng Lu, Xiao Cheng Zeng, Yinsheng Guo
Summary: This study directly visualizes ferroelastic twin domains in lead halide perovskites and demonstrates their role as internal reflectors for energy transport. The findings show that these domain walls have low energies and can easily switch between different orientations, making them suitable for optical guiding of internal photoexcitations.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yangyan Gao, Xin He, Keke Mao, Christopher K. Russell, Sam Toan, Aron Wang, TeYu Chien, Fangqin Cheng, Armistead G. Russell, Xiao Cheng Zeng, Maohong Fan
Summary: Commercial single-walled carbon nanotubes (CNTs) were activated with nitric acid and urea under ultrasonication and hydrothermal methods, respectively, to prepare N-doped CNTs with -COOH functional groups. The chemically modified CNTs catalyze both CO2 sorption and desorption, with significant increases in desorption rate compared to the sorbent without the catalyst.
Article
Chemistry, Multidisciplinary
Yuan Liu, Jian Jiang, Yangyang Pu, Joseph S. Francisco, Xiao Cheng Zeng
Summary: The study investigates the freezing transition of water confined in double-walled carbon nanotubes using large-scale molecular dynamics simulations. The results show that water can spontaneously form single-walled ice nanotubes with diameters up to 10 nm. Three different types of ice nanotubes are observed. Ab initio molecular dynamics simulations are also performed to examine the stability of the ice nanotubes.
Article
Chemistry, Multidisciplinary
Qun Ji, Yilei Wu, Xinying Gao, Tingbo Zhang, Yipeng Zhou, Yehui Zhang, Ming-Gang Ju, Jinlan Wang, Xiao Cheng Zeng
Summary: Tin organic-inorganic halide perovskites (tin OIHPs) have a desirable band gap and their power conversion efficiency (PCE) has reached 14%. It was previously believed that the organic cations in tin OIHPs had little impact on the optoelectronic properties. However, we found that defective organic cations with randomly dynamic characteristics do have a significant effect on the optoelectronic properties of tin OIHPs.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Biwu Chu, Yuan Liu, Hao Li, Yongcheng Jia, Jun Liu, Qing Cao, Tianzeng Chen, Peng Zhang, Qingxin Ma, Xiao Cheng Zeng, Joseph S. Francisco, Hong He
Summary: Using a flow tube reactor, it was discovered that N2O5 can be released from the TiO2 surface during the photocatalytic oxidation of NO2, which provides a previously unreported source of N2O5. The release rate of N2O5 from TiO2 depends on various factors including the initial NO2 concentration, relative humidity, O-2/N-2 ratio, and irradiation intensity. Experimental and theoretical studies show that this release is due to the reaction of NO2 with surface hydroxyl groups and electron holes on TiO2, followed by its combination with another NO2 molecule to form N2O5.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Rui Zhang, Wenshan Liu, Feng-Ming Zhang, Zhao-Di Yang, Guiling Zhang, Xiao Cheng Zeng
Summary: COF-C4N was found to be an effective oxygen evolution reaction (OER) electrocatalyst with low overpotential, and it has ideal N-edge cavities suitable for anchoring transition metal (TM) sites, thereby achieving higher OER activity as single atom catalysts (SACs). Two descriptors for characterizing the OER activities were proposed based on density-functional theory calculations, and Co-COF-C4N and Ni-COF-C4N were theoretically suggested to be highly active and low-cost OER SACs for target synthesis.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Jiaqi Lin, Jiaxin Jiang, Jiaqi Zhang, Hongyan Guo, Xiao Cheng Zeng, Zhiwen Zhuo, Ning Lu
Summary: A new diamond-like boron carbonitride material (BC6N) with excellent mechanical, electronic, and optical properties has been discovered. It can be synthesized easily and has potential applications as a superhard and high-temperature material, as well as in the semiconductor and optical devices fields.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Zhongjun Li, Yahui Zheng, Guojun Li, Hanxi Wang, Weiduo Zhu, Haidi Wang, Zhao Chen, Yupeng Yuan, Xiao Cheng Zeng, Yucheng Wu
Summary: The deviation of the Schottky barrier (SB) in the ultraclean van der Waals contact between 2D MoS2 and 3D In from the Schottky-Mott limit (SML) is investigated. The deviation is found to be attributed to the combined effects of interface potential difference (?V) and Fermi-level shift (?E-F). By coating a thin film of Au, Sc, or Ti on the back side of In, the deviation and the sum of ?V and ?E-F can be reduced. Particularly, the SB is significantly reduced to 0.12 eV in the Ti coating case. This interface engineering can be applied to regulate the SB between a 2D semiconductor and a 3D alloy.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Bo Lin, Jian Jiang, Xiao Cheng Zeng, Lei Li
Summary: Understanding the phase behavior of nanoconfined water films is important in various fields. This study developed a machine-learning force field to determine the phase diagram of monolayer water/ice in nanoconfinement. Two new high-density ices were discovered, with unique hydrogen-bonding networks. The study also identified the stable region for the lowest-density monolayer ice at negative pressures.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Yaxin Gao, Sha Li, Xiao Cheng Zeng, Menghao Wu
Summary: In this study, it is found that valence stratification can cause symmetry breaking and generate ferroelectricity in two-dimensional materials. The monolayer Cu2Cl3 structure with stratified Cu ions into Cu(i) and Cu(ii) layers is obtained through ab initio computation. This unique monolayer not only has lower formation energy than the bulk CuCl + CuCl2, but also exhibits a previously unreported chemical valencing phenomenon through vertical ferroelectric switching. Moreover, the Jahn-Teller distortion of the Cu(ii) layer results in in-plane ferroelectricity and the monolayer's ferroelasticity and ferromagnetism are coupled with in-plane and vertical polarization, respectively, leading to the emergence of 2D triferroicity and triferroic couplings.
Article
Chemistry, Physical
Zhongjun Li, Yahui Zheng, Guojun Li, Hanxi Wang, Weiduo Zhu, Haidi Wang, Zhao Chen, Yupeng Yuan, Xiao Cheng Zeng, Yucheng Wu
Summary: The Schottky barrier (SB) in the van der Waals contact between MoS2 and indium deviates from the Schottky-Mott limit (SML). The deviation is attributed to the combined effects of interface potential difference (Delta V) and Fermi-level shift (Delta EF). Coating a thin film of Au, Sc, or Ti on the back side of indium can mitigate the SB deviation and decrease Delta V and Delta EF. Notably, the Ti coating reduces the SB to 0.12 eV, smaller than the value in the Au coating case.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Ning Lu, Xin Hu, Jiaxin Jiang, Hongyan Guo, Gui Zhong Zuo, Zhiwen Zhuo, Xiaojun Wu, Xiao Cheng Zeng
Summary: In this study, the structural stability and electronic properties of point defects in α-antimonene were investigated through first-principles calculations. Compared to analogs like phosphorene, graphene, and silicene, most defects in α-antimonene can be easily generated. Among the nine types of point defects, the single vacancy SV-(5|9) is likely the most stable, with a concentration higher than that in phosphorene. Additionally, the vacancy exhibits low diffusion barriers in the zigzag/armchair direction.
