Tuning Nanoparticles and Nanostructures to Deliver Unprecedented Catalytic Activity for CO₂ Conversion into Fuels, CO Oxidation and Clean Hydrogen Production

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Our group explores tuning nanoparticles’ sizes, shapes and compositions to achieve the highest catalytic activity. This effort includes novel synthesis of nm and sub-nm metal nanoparticles coupled with studies of their interfacial chemistry in model and applied catalytic systems. Recent discoveries include striking (almost 2 orders of magnitude) improvement of catalytic hydrogen production from water using sub-nm Au nanoparticles. Our collaborative efforts also resulted in development of a new method for nanoparticulate catalyst synthesis utilizing He droplets templating.

Representative Publications:

Haotian Yang, Jiajie Cen, Qiyuan Wu, Claron J. Ridge, Xiao Tong, Chenyu Zhou, Vijayen Veerasamy, Dong Su, C. Michael Lindsay, Mingzhao Liu*, and Alexander Orlov* "Enhancing CO Oxidation Activity via Tuning a Charge Transfer Between Gold Nanoparticles and Supports", J. Phys. Chem. C, 2022, 126, 4836.
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[Highlighted by SBU newsroom] DOI:10.1021/acs.jpcc.1c10072

Qiyuan Wu, Binhang Yan, Jiajie Cen, Janis Timoshenko, Dmitri N. Zakharov, Xianyin Chen, Huolin Xin, Siyu Yao, John B. Parise, Anatoly I. Frenkel, Eric A. Stach, Jingguang G. Chen*, and Alexander Orlov*, "Growth of Nanoparticles with Desired Catalytic Functions by Controlled Doping-Segregation of Metal in Oxide", Chemistry of Materials, 2018, 30, 1585.
DOI:10.1021/acs.chemmater.7b04699

Qiyuan Wu, Claron J. Ridge, Shen Zhao, Dmitri Zakharov, Jiajie Cen, Xiao Tong, Eoghan Connors, Dong Su, Eric A. Stach, C. Michael Lindsay*, and Alexander Orlov*, "Development of a New Generation of Stable, Tunable, and Catalytically Active Nanoparticles Produced by the Helium Nanodroplet Deposition Method", J. Phys. Chem. Lett., 2016, 7, 2910.
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DOI:10.1021/acs.jpclett.6b01305

Computational Design and Synthesis of Novel Photocatalytic Materials for Clean Energy

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Our group is developing novel catalysts to: (a) remove water and gas phase contaminants, (b) produce hydrogen via photocatalytic water splitting and (c) transform CO2 into fuels via photoreduction. Our projects include research funded by Materials Genome Initiative (under the White House OSTP) to facilitate theory driven design of novel photocatalysts. The recent discoveries include the very first synthesis of GaN-ZnO catalysts under high pressures and temperatures, where hydrogen production was achieved with no sacrificial reagents or co-catalysts. We also focus on scaling up synthesis of catalysts and large scale applications of photocatalysis.

Representative Publications:

Jiajie Cen, Qiyuan Wu, Danhua Yan, Wenrui Zhang, Yue Zhao, Xiao Tong, Mingzhao Liu*, Alexander Orlov*, "New aspects of improving the performance of WO3 thin films for photoelectrochemical water splitting by tuning the ultrathin depletion region", RSC Advance, 2019, 9, 899.
DOI:10.1039/c8ra08875f

Jiajie Cen, Qiyuan Wu, Mingzhao Liu*, Alexander Orlov*, "Developing New Understanding of Photoelectrochemical Water Splitting via in-situ Techniques: A Review on Recent Progress", Green Energy & Enviroment, 2017, 2, 100.
DOI:10.1016/j.gee.2017.03.001

Observing Chemical Reactions and Nanoparticle Growth in Catalytic, Energy Storage, Electrochemical and Photo Electrochemical Systems : in-situ XANES, E-TEM, XRD, XPS, XAS and DRIFTS Studies

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Our efforts include design and applications of unique in-situ spectroscopic characterization techniques for studies of catalysts, adsorbents and polymer/nanofiller interfaces. These techniques include in-situ DRIFTS modified with UV source, in-situ XRD-DSC and environmental TEM (E-TEM). One of the unique aspects of our research is in utilization of a new generation of E-TEM chips, which we modify with oxide films to study supported cluster mobility under reaction conditions. In collaboration with our BNL colleagues we also utilize in-situ EXAFS and XANES techniques, where we study catalysts under reaction conditions. These efforts can lead to better understanding the reaction mechanisms and catalyst’s behavior for gas and liquid phase reactions.

Representative Publications:

Li, S., Yao, Z., Zheng, J., Fu, M., Cen, J., Hwang, S., Jin, H., Orlov, A., Gu, L., Wang, S., Chen, Z., Su, D., "Direct observation of defect‐aided structural evolution in Ni‐rich layered cathode", Angewandte Chemie, 2020, 132, 2-10.
DOI:10.1002/anie.202008144

Hwang, S., Meng, Q., Chen, P-F., Kisslinger, K., Cen, J., Orlov, A., Zhu, Y., Stach, E. A., Chu, Y-H., Su, D., "Strain Coupling of Conversion-type Fe₃O₄ Thin Film for Lithium Ion Battery", Angewandte Chemie, 2017, 129, 7921-79024.
DOI: 10.1002/ange.201703168

Ramakrishnan, G., Zhao, S., Han, W., Orlov, A., , "Simultaneous observation of gas phase and surface species in photocatalytic reactions on nanosize Au modified TiO₂: The next generation of DRIFTS systems", Chemical Engineering Journal, 2011, 170, 445-450.
DOI:10.1016/j.cej.2010.12.003

Transforming Solar Industry by Creating A New Generation of Self-cleaning Solar Panels for Desert Regions

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Based on NASA heritage technology our group has developed a new generation of ElectroDynamic Shield (EDS) technology that can clean solar panels at scale. This work has been recognized by R&D100 Award, often referred to as "Oscar of Innovation".

Transforming Polymer Composites and Structural Concrete into More Sustainable and Environmentally Friendly Materials

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Our latest work demonstrated how concrete, the largest material humanity manufactures can be made more environmentally friendly by adsorbing air pollutants. Our efforts are also focused on design of better polymer-nanomaterials composites by understanding the mechanisms of nanomaterials release from polymer matrices. Both qualitative and quantitative understanding of these mechanisms can aid in designing more sustainable ‘green’ polymer nanocomposites. For example, in our work highlighted by the EU Commission, we elucidated several aspects of nanomaterials release and toxicity from epoxy composites..

Representative Publications:

Ariyachandra, E., Patel, PS., Orlov, A., Peethamparan, S., "Effect of NO2 sequestered Recycled Concrete Aggregate (NRCA) on Mechanical and Durability Performance of Concrete", Cement and Concrete Research, 2020, 137, 106210.
DOI:10.1016/j.cemconres.2020.106210

Ramakrishnan, G., Orlov, A., "Development of novel inexpensive adsorbents from waste concrete to mitigate NOx emissions", Building and Environment, , 2014, 72, 28-33.
DOI:10.1016/j.buildenv.2013.10.016

James Ging, Raul Tejerina-Anton, Girish Ramakrishnan, Mark Nielsen, Kyle Murphy, Justin M. Gorham, Tinh Nguyen, Alexander Orlov*, "Development of a conceptual framework for evaluation of nanomaterials release from nanocomposites: Environmental and toxicological implications", Science of the Total Environment, , 2014, 473, 9-19...
DOI:10.1016/j.scitotenv.2013.11.135