Huang, Liangliang

Molecular simulation is an important research tool that gives us an ever-increasing ability to predict the physical and chemical properties of matter, as well as to design and engineer novel materials and efficient processes. The importance of molecular simulation is evidenced by several recent reports from funding agencies in the U.S., which emphasize the rapidly growing value of simulation in the fields of chemistry, chemical engineering, material science, physics, medical and bio-related disciplines. We have had dramatic increases in the power and availability of high- performance computers; in parallel with these developments, increasingly robust and efficient algorithms and simulation methods have been developed, with the ability to integrate quantum mechanical calculations, atomistic Monte Carlo and molecular dynamics simulations, mesoscale and continuum approaches. The combination of multi-scale modeling techniques gives us an unprecedented ability to accurately estimate the properties of complex materials and systems, as well as to aid in the interpretation of experimental results. Our group will use theory and multi-scale molecular modeling methods and collaborate with experimental groups for two main goals:

- understanding the behavior and controlling factors for complex surfaces and structures of relevance in biomedical and catalytic systems;
- carrying out computer-aided discovery and design of new materials and structures;
Achieving such general objectives would have a positive impact on society, giving us new ways to treat diseases such as cancer and diabetes, to improve the accuracy and sensitivity of biosensors,to design materials for the removal of pollutants in the environment or detect and capture potential chemical or biological warfare agents, and to reduce the production costs of catalytic processes and of chemicals and pharmaceutical products, among others.
Current Research Interest:

1. Biofunctionalization of Graphene Oxide Surface for Drug Delivery:

Graphene oxide (GO) exhibits unique 2-D structure and exceptional physical, chemical and optical properties that lead to many potential biomedical applications. In the last few years, GO has attracted increasing interest as a molecular carrier for in vitro and in vivo drug delivery. It is also accepted that functionalization of GO sheets must be conducted to attain high biocompatibility. Results have shown that well-functionalized GO sheets are stable and safe for in vitro drug delivery, and that they can be readily excreted through the renal route and are non- toxic in vivo to mice.From the molecular point of view, the carbonyl, epoxy, hydroxyl and other oxygen functional groups on the basal planes and edges of GO sheets significantly alter their van der Waals and electrostatic interactions compared to those on pristine graphene. This explains why GO can immobilize a large number of substances, including metals, drugs, biomolecules and fluorescent molecules. However, there is still no systematic study on GO functionalization and we do not know the fundamental mechanisms that underlie the design of the GO surface to achieve simultaneously high loading capacity, high sensitivity and high biocompatibility for drug delivery purposes.To aid the integration of GO into clinical drug delivery and other biomedical applications, We are interested in applying and improving multi-scale modeling techniques to address the following challenges:
(1) An efficient method of GO functionalization for high biocompatibility and low toxicity. It is accepted that biofunctionalization can integrate GO with biomolecules, such as nucleic acids, peptides and proteins, and that the GO derivatives bind with the drug molecules through non-covalent interactions.
(2) Smart functionalization to increase targeting efficiency of GO-based drug carrier systems. It is of fundamental advantage to develop delivery systems with a molecular-recognition strategy, in which the therapeutic agents are carried with recognition capacity and optical, fluorescent or electric signals for imaging analysis. It is also important to develop functionalization methods so that the GO–based nano-materials are biodegradable in physiological systems after delivering the drugs.
(3) The interaction mechanisms of GO-drug complexes in physiological systems, for example, the in vivo behaviors of GO-based nanomaterials, the intracellular uptake mechanisms and the intracellular metabolic pathway. As illustrated in Figure 2, the three challenges require an understanding of covalent interactions between GO and the functionalization polymers or molecules, and of non-covalent interactions between the GO-based nano-materials with the physiological systems, for example, proteins, DNA, peptides, cells, drugs or bacteria.

2. Mesoporous Titanium Dioxide for Reaction and Mass Transport:

The study of heterogeneous catalysis has bred four Nobel Prizes in Chemistry, Fritz Haber in 1918, Carl Bosch and Friedrich Bergius in 1931, Irving Langmuir in 1932, and Gerhard Ertl in 2007. It is of paramount importance in the chemical, biomedical and materials industries, and the field needs a continuous focus and efforts. In the heterogeneous catalysis process, the phase of the catalyst differs from that of the reactants. In general, the reactants diffuse from the bulk to the catalyst surface, adsorb and form new chemical bonds with the catalytic sites, and then desorb and diffuse from the surface after the reactions. We need fundamental understanding of: (1) the diffusion, adsorption, chemical reaction mechanisms and the mass transport phenomena of the reactants; (2) the properties of the catalytic surface and how to select, optimize and design support materials for different catalysts and different applications.
This fundamental understanding is difficult to achieve from experiments alone, since the measurements reflect a sum of many effects – diffusion, selective adsorption of particular reactants or products, chemical kinetic limitations, activity and stability of catalyst, effects of support material defects and roughness, etc. Theoretical studies can play an important part in determining the role of these many factors, and in achieving both fundamental understanding and fine control of these effects. Titanium dioxide material has been widely studied as a heterogeneous photocatalyst for environmental applications, for example the degradation of organic pollutants and the dye- sensitized solar cell. Due to the in vivo biocompatibility, it also finds application in human osteoblasts and other implant materials. Recently, Crossland and the co-workers reported an enhanced mobility and optoelectronic performance on mesoporous anatase TiO2 single crystals. This is because mesoporous anatase TiO2 provides both the desired large surface area and the long-range electronic connectivity and structural coherence. We recently examined the TiO2 surface activity by studying water dissociation on different TiO2 facets, and the ReaxFF molecular dynamics simulation results showed that the TiO2-B (100) is the most active but stable facet for water dissociation, and that the activity difference can be explained by the surface density of unsaturated Ti sites and the geometric surface curvature. For this project, we plan to collaborate with experimental groups on this project, to use mesoporous titanium dioxide material and study the simultaneous adsorption, diffusion and reactions of water (H2O), ammonia (NH3) and acetic acid (CH3COOH) for the following objectives:
(1) To develop a ReaxFF force field to describe both the mesoporous TiO2 structure and the reactive interactions between the fluids and TiO2 surfaces;
(2) To develop a coarse- grained model for mesoporous TiO2 structure;
(3) To perform a suite of theory and simulation methods, spanning the electronic, atomistic and mesoscale of matter, to treat simultaneous adsorption, diffusion and chemical reaction in mesoporous TiO2 catalysts. The methods will be able to predict the reaction mechanism and rate, the reaction effects on adsorption and diffusion of reactants and the stability of mesoporous TiO2 surface features;
(4) To apply these methods to study ammonia and acetic acid dissociations on the mesoporous TiO2 catalysts;
(5) To study and design mesoporous TiO2 materials, with optimized reaction-diffusion characteristics, controllable surface hydrophobicity and hydrophilicity, and a desirable surface friction property.  

Shanshan Wang, Haiming Wang, Zhibin Su, Liangliang Huang, Xiaojing Guo, Zhongyang Dai, Yudan Zhu, Wei ZHuang, Linghong Lu, Xiaohua Lu, “Computational Screening Carbon- Based Adsorbents for CH4 Delivery Capacity”, Fluid Phase Equilibria, 2019, 494, 184-191.

Mohamed Mehana, Mashhad Fahes, Liangliang Huang, “Asphaltene Aggregation in Oil and Gas Mixtures: Insights from Molecular Simulation”, Energy & Fuels, 2019, accepted.

Hao Xiong, Deepak Devegowda, Liangliang Huang, "EOR Solvent-Oil Interaction in Clay- Hosted Pores: Insights from Molecular Dynamics Simulations", Fuel, 2019, 249, 233-251.

Xiaobao Li, Yanian Gao, Xiaolong Zhou, LiCheng Li, Liangliang Huang, Judi Ye, Tianyang Zhang, “Nano-ZnO/Regenerated Cellulose Films Prepared by Low-temperature Hydrothermal Decomposition of Zn5(OH)8Cl2·H2O from Cellulose-ZnCl2 Aqueous Solution”, Materials Letters, 2019, 245(15), 82-85.

Li Li, Guobing Zhou, Zhen Yang, Fang Fang, Qi Qiao, Na Hu, Liangliang Huang, Xiangshu Chen, “Molecular-Level Understanding of Translational and Rotational Motions of C2H6, C3H8, n-C4H10 and Their Binary Mixtures with CO2 in ZIF-10”, Journal of Chemical & Engineering Data, 2019, 64(2), 484-496. (Supplementary Cover)

Li Liu, Fan Pan, Chang Liu, Liangliang Huang, Wei Li, Xiaohua Lu, “TiO2 Nanofoam-Nanotube Array for Surface-Enhanced Raman Scattering”, ACS Applied Nano Materials, 2018, 1(12), 6563-6566.

Qi Qiao, Chang Liu, Wei Gao, Liangliang Huang, “Graphene Oxide Model with Desirable Structural and Chemical Properties”, Carbon, 2019, 143, 566-577.

Xiaolong Zhou, Xiaobao Li, Yanian Gao, Licheng Li, Liangliang Huang, Judi Ye, “Preparation and Characterization of 2D ZnO Nanosheets/Regenerated Cellulose Phiticatalytic Composite Thin Films by A Two-Step Synthesis Method”, Materials Letters, 2019, 234(1), 26-29.

Wei Cao, Liangliang Huang, Ming Ma, Linghong Lu, Xiaohua Lu, “Water in Narrow Carbon Nanotubes: Roughness Promoted Diffusion Transition”, Journal of Physical Chemistry C, 2018, 122, 33, 19124-19132.

Jinxia Zhou, Liangliang Huang, Wei Yan, Jun Li, Chang Liu and Xiaohua Lu, “Theoretical Study of the Mechanism for CO2 Hydrogenation to Methanol Catalyzed by trans-RuH2(CO) (dpa)”, Catalysts, 2018, 8(6), 244.

Rong An, Guobing Zhou, Yudan Zhu, Wei Zhu, Liangliang Huang and Faiz Ullah Shah, “Friction of Ionic Liquid-Glycol Ether Mixtures at Titanium Interfaces: Negative Load Dependence”, Advanced Materials Interfaces, 2018, 5(14), 1800263. (Front Cover).

Lu Tan, Liangliang Huang, Yingchun Liu and Qi Wang, “Augmented Pairwise Addition Model for Lateral Adsorbate Interactions: the NO-CO Reaction System on Rh(100) and Rh(111)”, Langmuir, 2018, 34(18), 5174-5183.

Guobing Zhou, Chang Liu and Liangliang Huang, “Molecular Dynamics Simulation of First Adsorbed Water Layer at Titanium Dioxide Surfaces”, Journal of Chemical & Engineering Data, 2018, 63(7), 2420-2429.

Lu Tan, Liangliang Huang, Qi Wang and Yingchun Liu, “Detailed Mechanism of the NO + CO Reaction on Rh(100) and Rh(111): A First-Principles Study”, Applied Surface Science, 2018, 444(30), 276-286.

Keith E. Gubbins, Kai Gu, Liangliang Huang, J. Matthew Mansell, Erik E. Santiso, Kaihang Shi, Małgorzata Śliwińska-Bartkowiak and Deepti Srivastava, “Surface-Driven High Pressure Processing”, Engineering, 2018, 4(3), 311-320.

Mohamed Mehana, Liangliang Huang and Mashhad Fahes, “The Density of Oil-Gas Mixtures: Insights from Molecular Simulations”, SPE Journal, 2018, Document ID: SPE-187297-PA, DOI: 10.2118/187297-PA

Licheng Li, Hanqin Yue, Shanshan Chen, Liangliang Huang, Xiaobao Li, Zhuhong Yang, Xiaohua Lu, “Interfacial Engineering of NiMo/Mesoporous TiO2 Catalyst with Carbon for Enhanced Hydrodesulfurization Performance”, Catalysis Letters, 2018, 148(3), 992-1002.

Dongxue Li, Kiros Hagos, Liangliang Huang, Xiaohua Lu, Chang Liu and Hongliang Qian, “Self-Propagating High-Temperature Synthesis of Potassium Hexatitanate Whiskers”, Ceramics International, 2017, 43, 17, 15505-15509.

Yihui Dong, Rong An, Shuangliang Zhao, Wei Cao, Liangliang Huang, Wei Zhuang, Linghong Lu and Xiaohua Lu, “Molecular Interactions of Protein with TiO2 by AFM Measured Adhesion Force”, Langmuir, 2017, 33(42), 11626-11634.

Lu Tan, Liangliang Huang, Qi Wang, Yingchun Liu, “A First Principles Study on O2 Adsorption and Dissociation Processes over Rh(100) and Rh(111) Surfaces”, Langmuir, 2017, 33(42), 11156-11163.

Li Li, Deshuai Yang, Trevor R. Fisher, Qi Qiao, Zhen Yang, Na Hu, Xiangshu Chen and Liangliang Huang, “Molecular Dynamics Simulations for Loading-Dependent Diffusion of CO2, SO2, CH4, and Their Binary Mixtures in ZIF-10: The Role of Hydrogen Bond”, Langmuir, 2017, 33(42), 11543-11553.

Rong An, Liangliang Huang, Kenneth P. Mineart, Yihui Dong, Richard J. Spontak and Keith E. Gubbins, “Adhesion and Friction in Polymer Films on Solid Substrates: Conformal Sites Analysis and Corresponding Surface Measurements”, Soft Matter, 2017, 13, 3492. (Back cover).

35. Wei Cao, Linghong Lu, Garrett M. Tow, Liangliang Huang, Tingting Yang and Xiaohua Lu, “Hydrophilicity Effect on CO2/CH4 Separation using Carbon Nanotube Membranes: Insights from Molecular Simulation”, Molecular Simulation, 2017, 43, 502-509.

Fu, Fangjia; Li, Yunzhi; Yang, Zhen; Zhou, Guobing; Huang, Yiping; Wan, Zheng; Chen, Xiang- Shu; Hu, Na; Li, Wei; Huang, Liangliang, “Molecular-Level Insights Into Size-Dependent Stabilization Mechanism of Au Nanoparticles in 1-Butyl-3-Methylimidazolium Tetrafluoroborate Ionic Liquid”, J. Phys. Chem. C, 2017, 121(1), 523-532.

Luchao Jin, Ahmad Jamili, Liangliang Huang and Felipe Perez, "Modeling the Mechanism of Clay Damage by Molecular Dynamics Simulation", Geofluids, 2017, 2017, 1747068.

Wei Cao, Linghong Lu, Liangliang Huang, Yihui Dong and Xiaohua Lu, "Molecular Behavior of Water on Titanium Dioxide Nanotubes: A Molecular Dynamics Simulation Study", J. Chem. Eng. Data, 2016, 61(12), 4131-4138.

Yaofeng Hu, Liangliang Huang, Shuangliang Zhao, Honglai Liu and Keith E. Gubbins, "Effects of Confinement in Nano-Porous Materials on the Solubility of a Supercritical Gas", Molecular Physics, 2016, 114(22), 3294-3306.

Jing Zheng, Junqiao Zhang, Lu Tan, Debing Li, Liangliang Huang, Qi Wang and Yingchun Liu, "Effects of Aspect Ratio on Water Immersion into Deep Silica Nanoholes", Langmuir, 2016, 32(34), 8759-8766.

Wei Cao, Garrett M. Tow, Linghong Lu, Liangliang Huang and Xiaohua Lu, "Diffusion of CO2/CH4 Confined in Narrow Carbon Nanotube Bundles", Molecular Physics, 2016, 114(16-17), 2530-2540.

Chang Liu, Yanhua Guo, Qiliang Hong, Chao Rao, Haijuan Zhang, Yihui Dong, Liangliang Huang, Xiaohua Lu and Ningzhong Bao, "Bovine Serum Albumin Adsorption in Mesoporous Titanium Dioxide: Pore Size and Pore Chemistry Effect", Langmuir, 2016. 32(16), 3995-4003.

Xiaobao Li, Xue Zhang, Licheng Li, Liangliang Huang, Wei Zhang, Judi Ye and Jianguo Hong, "Low-Temperature Hydrothermal Synthesis of ZnO/Regenerated Cellulose Nanocomposite", Materials Letters, 2016, 175, 122-125.

Guobing Zhou, Yunzhi Li, Zhen Yang, Fangjia Fu, Yiping Huang, Zheng Wan, Li Li, Xiangshu Chen, Na Hu and Liangliang Huang, "Structural Properties and Vibrational Spectra of Ethylammonium Nitrate Ionic Liquid Confined in Single-Walled Carbon Nanotubes", J. Phys. Chem. C, 2016, 120(9), 5033-5041.

Rong An, Liangliang Huang, Yun Long, Berc Kalanyan, Xiaohua Lu and Keith E Gubbins, "Liquid-Solid Nano-friction and Interfacial Wetting", Langmuir, 2016, 32(3), 743-750.

Chang Liu, Jun Wang, Xiaoyan Ji, Liangliang Huang and Xiaohua Lu, "The Biomethane Producing Potential in China: A Theoretical and Practical Estimation", Chinese Journal of Chemical Engineering, 2016, 24(7), 920-928.

Xiaojing Guo, Guozhong Wu, Cheng Li, Hengfeng Gong, Jiangtao Hu, Chan Jin, Liangliang Huang and Ping Huai, "DFT Investigations of Uranium Complexation with Amidoxime-, Carboxyl- and Mixed Amidoxime/Carboxyl-based Host Architectures for Sequestering Uranium from Seawater", Inorganica Chimica Acta., 2016, 441, 117-125.

Chang Liu, Nanhua Wu, Jun Wang, Liangliang Huang and Xiaohua Lu, "Determination of the Ion Exchange Process of K2Ti4O9 Fibers at Constant pH and Modeling with Statistical Rate Theory", RSC Adv., 2015, 5, 73474-73480.

Xiaojing Guo, Liangliang Huang, Cheng Li, Jiangtao Hu, Guozhong Wu and Ping Huai, "Sequestering Uranium from UO2(CO3)34- in Seawater with Amine Ligands: Density Functional Theory Calculations", Phys. Chem. Chem. Phys., 2015, 17, 14662-14673.

Liangliang Huang and Keith E. Gubbins, “Ammonia Dissociation on Graphene Oxide: An ab initio Density Functional Theory Calculation”, Z. Phys. Chem., 2015, 229, 1211-1223.

Liangliang Huang, Keith E. Gubbins, Licheng Li and Xiaohua Lu, “Water on Titanium Dioxide Surface: A Revisit by Reactive Molecular Dynamics Simulations”, Langmuir, 2014, 30, 14832.

Long Chen, Liangliang Huang, and Jiahua Zhu, “Stitch Graphene Oxide Sheets into Membrane at Liquid/Liquid Interface”, Chem. Commun., 2014, 50, 15944.

Wei Cao, Linghong Lu, Liangliang Huang, Shanshan Wang, and Yudan Zhu, “Molecular Simulations on Diameter Effect of Carbon Nanotube for Separation of CO2/CH4”, CIESC J., 2014, 65, 1736.

"Controllable Atomistic Graphene Oxide Model and its Application in Hydrogen Sulfide Removal", Liangliang Huang, Mykola Seredych, Teresa J. Bandosz, Adri C. van Duin, Xiaohua Lu and Keith E. Gubbins, Journal of Chemical Physics, 139, 194707, 2013.

"Reactive Adsorption of Ammonia and Ammonia/Water on CuBTC Metal-Organic Framework: a ReaxFF Molecular Dynamics Simulation", Liangliang Huang, Teresa J. Bandosz, Kaushik L. Joshi, Adri C. T. van Duin, and Keith E. Gubbins, Journal of Chemical Physics, 138,034102, 2013.

"ReaxFF Molecular Dynamics Simulation of Thermal Stability of a Cu3(BTC)2 Metal-Organic Framework", Liangliang Huang, Kaushik L. Joshi, Adri C. T. van Duin, Teresa J. Bandosz, and Keith E. Gubbins, Physical Chemistry Chemical Physics, 14, 11327, 2012.

“Towards Understanding Reactive Adsorption of Ammonia on Cu-MOF/Graphite Oxide Nanocomposites”, Camille Petit, Liangliang Huang, Jacek Jagiello, Jeffrey Kenvin, Keith E. Gubbins, and Teresa J. Bandosz, Langmuir, 13043, 27, 2011.

“Melting Behavior of Bromobenzene within Carbon Nanotubes”,M. Sliwinska-Bartkowiak, M. Jazdzewska, Keith E. Gubbins and Liangliang Huang, J. Chemical Engineering Data, 55, 4183, 2010.

“Melting Behavior of Water in Cylindrical Pores: Carbon Nanotubes and Silica Glasses”, M. Sliwinska-Bartkowiak, M. Jazdzewska, Liangliang Huang and Keith E. Gubbins, Physical Chemistry Chemical Physics, 10, 4909,2008.

“Simulations of Binary Mixture Adsorption of Carbon Dioxide and Methane in Carbon Nanotubes: Temperature, Pressure, and Pore Size Effects”,Liangliang Huang, Luzheng Zhang, Qing Shao, Jun Wang, Linghong Lu, Xiaohua Lu, Shaoyi Jiang, and Wenfeng Shen, Journal of Physical Chemistry C, 111, 11912, 2007.

“Helicity and temperature effects on static properties of water molecules confined in modified carbon nanotubes”, Liangliang Huang, Qing Shao, Linghong Lu, Xiaohua Lu, Luzheng Zhang, Jun Wang, and Shaoyi Jiang, Physical Chemistry Chemical Physics, 8, 3836, 2006.