(2bc) Design of Heterogeneous Catalysts for Energy Conversion Reactions

The extensive use of fossil fuels in the development of global economy and industrialization has created severe problems in our society including climate change, energy crisis, global warming, pollution, etc. Electrochemical energy conversion reactions such as water splitting, CO₂ reduction reaction (CO₂RR), and NO₃ reduction reaction (NO₃RR) provide an alternative way for renewable and sustainable developments. These reactions have a high reaction barrier under normal atmospheric conditions, demanding an appropriate electrocatalyst to lower the reaction barrier. Transition metal (TM) based heterogeneous catalysts have emerged as potential candidates for electrochemical reaction due to their flexible structural behavior for optimizing the activities and convenience to build appropriate model systems for investigating the reaction mechanism. The primary goal of my research will be the development of a highly active and durable heterogeneous electrocatalyst via computational methodology including density functional theory (DFT), Machine Learning (ML) with experimental collaboration. In order to design highly effective heterogeneous catalysts, I will first use our recently developed Grand Canonical Potential Kinetics (GCP-K) method using first-principles DFT calculation to predict free energies, to identify active site, reaction mechanism, kinetics, stability, and electronic properties-activity relationship. Through high throughput screening using feature vectors combined with deep neural networks, a supervised and unsupervised Machine Learning (ML) technique will be established to determine the catalyst's performance, including activity and selectivity, and their link with structure. Then, through a highly skilled experimental teamwork, we will generate the highly active and long-lasting catalysts we have projected. My main areas of interest will be the design of materials and the process optimization of electrochemical conversion reactions. As a result of my prior experience, I have a great deal of faith that by combining cutting-edge computational methods with effective methods for fabricating and analyzing materials, we will be able to create highly active, effective, and stable heterogeneous electrocatalysts for electrochemical conversion reactions.

Ph.D. Research Summary

Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Hong Kong; Advisor: Prof. Zhengtang Luo

Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA, 91125, USA; Advisor: William A. Goddard (III)

During working with Prof. Zhengtang Luo, I used both computational chemistry and experimental validation techniques to understand the origin of single-atom catalysts (SACs) activity toward hydrogen evolution reaction. Our systematic study elucidates the fundamental understanding for the designing of highly selective SACs for HER [1]. Later part of my Ph.D., I developed a constant potential-based grand canonical potential kinetics (GCP-K) method for the CO2RR along with Prof. William A. Goddard, at Caltech [2]. We extended our method to other 2D materials other than the CO2RR reaction [3]. I studied the thermal behavior of carbon electrodes using the LAMMPS simulation technique [4]. I was actively involved in mentoring junior graduate students and collaborated on several exciting and interesting projects across the world during my Ph.D. period [5-7].

Current Postdoctoral Research

SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University and SLAC National Accelerator Laboratory, CA 94305, United States; Advisor: Michal Bajdich and Frank Abild-Pedersen

My postdoctoral research focuses on designing heterogeneous electrocatalysts for electrochemical reactions such as water splitting, NO₃RR, CO₂RR, etc. Spin transition in metal during electrocatalysis plays a significant role in predicting electrochemical activities. I used VASP and ORCA codes to predict hyperfine isotropic coupling constant for different planar and non-planar M-N₄-based SACs geometry. I found empty Ni²⁺-SAC highly stable at high spin state due to the transition of square planar geometry (D_4h symmetry) of Ni-N₄ moiety into distorted tetrahedral geometry (D_2d symmetry), which is further confirmed experimentally by ⁶¹Ni Mossbauer Spectroscopy characterization [8]. Further, I extend spin-transition chemistry research for other SACs (Mn, Co, Fe) towards OER/ORR as a function of constant applied potential using the GCP-K method. Recently, I have developed a computationally feasible TM-based spinel-type high entropy oxide (HEO) impurity model to study stability, local strain, and its effect on OER activity followed by experimental validation [9]. This work illustrates the potential of HEO as a tunable property material due to its large number of stable thermodynamic configurations and local strain, which leads to a broad distribution of possible local electronic structures. Besides, I am actively involved in several ongoing exciting projects including NO₃RR, Benzyl Alcohol Oxidation (BAO), etc with experimental collaborations. I hope these experiences will guide me in bottom-up catalyst design for electrochemical applications in sustainable developments.

Selective Publications (Complete list of publication: https://scholar.google.com/citations?user=cwPYsMQAAAAJ&hl=en)

1. D. Hossain, Z. Liu, M. Zhuang, X. Yan, Gui-L. Xu, C. A. Gadre, X. Pan, K. Amine, Z. Luo*; Rational Design of Graphene‐Supported Single Atom Catalysts for Hydrogen Evolution Reaction; Advanced Energy Materials, 1803689, 2019.
2. D. Hossain, Y. Huang, T. H. Yu, W. A. Goddard III* and Z. Luo*; Reaction Mechanism and Kinetics for CO₂ Reduction on Nickel Single Atom Catalysts from Quantum Mechanics; Nature Communications 11 (1), 1-14, 2020.
3. D. Hossain^#, Z. Liu^#, H. Liu, A. Tyagi, F. Rehman, J. Li, M. Amjadian, Y.Cai, W. A Goddard III*^, and Z. Luo*; The Kinetics and Potential Dependence of the Hydrogen Evolution Reaction Optimized for the Basal Plane Te Vacancy Site of MoTe₂ from Theory and Experiment (Under review Nature Communications) (^# Equal contributions)
4. D. Hossain, Q. Zhang, T. Cheng, W. A. Goddard III*, Z. Luo*, Graphitization of low-density amorphous carbon for electrocatalysis electrodes from ReaxFF reactive dynamics, Carbon 183, 2021, 940-947.
5. Siddharth, P. Alam, M. D. Hossain, N. Xie, G. S. Nambafu, F. Rehman, Z. Luo, G. Chen, B. Z. Tang*, and M. Shao*; Hydrazine Detection during Ammonia Electro-oxidation Using an Aggregation-Induced Emission Dye; Journal of the American Chemical Society 143 (5), 2433-2440
6. Zhao, M. D. Hossain, C. Xu,Z. Lu, Yi-S. Liu, S.-H. Hsieh, I. Lee, Z.Luo, X. Duan, X. Pan, F. Zaera,J. Guo, W. A. Goddard III,Y. Huang*; Tailoring a three-phase microenvironment for high-performance oxygen reduction reaction in proton exchange membrane fuel cell, Matter, 3, 1-7, 2020.
7. Tamtaji, H. Gao, M. D. Hossain, P. R. Galligan, H. Wong, Z. Liu, H. Liu, Y. Cai, W.A. Goddard III and Z. Luo*; Machine Learning for Design Principles for Single Atom Catalysts towards Electrochemical reactions, Journal of Material Chemistry A 8, 2022.
8. M. Koshy, M. D. Hossain, R. Masuda, Y. Yoda, L. B. Gee, K.Abiose, A. Gallo, C. Hahn, M. Bajdich*, Z. Bao*, T. Jaramillo*; Investigation of the structure of atomically dispersed NiN_x sites in Ni, N-doped carbon electrocatalysts by ⁶¹Ni Mössbauer Spectroscopy and Simulations (Under Review)
9. Baek^#, M. D. Hossain^#, P.Mukherjee, J. Lee, K. T Winther, J. Leem, Y. Jiang, Hyun S.Jung, W. Chueh, M. Bajdich^*, and X. Zheng^*; Design of Spinel High Entropy Oxides for Oxygen Evolution Reaction: Theory and Experiment (Under review) (^# Equal contributions)

Teaching Statements

Teaching and mentorship are vital to the practice of research and have had a significant impact on my scientific education and my motivation to work in academia. My teaching experience has led me to the conclusion that a well-organized, interesting lecture needs to have the following elements: i) a clear statement of the lecture's main topic; ii) numerous examples used to illustrate the main points; and iii) a repetition of the take-home message at the end of the lecture. I strongly favor teaching core techniques and ideas above memorizing of facts and formulas. I have experience instructing Chemical Engineering courses such as Separation Processes (CENG 3210) and Nanomaterials Application in Chemical Engineering (CENG 5840) as teaching assistant (TA) during my Ph.D. period in HKUST, Hong Kong. At Stanford, I have participated in the teaching and mentoring workshop, graduate course design workshop, which helped me refine my methods for creating learning objectives, judging students fairly, and creating a welcoming classroom environment. During my Ph.D., I mentored five M.Sc./M.Phil. and 3 new graduate students, specially students from under-represented backgrounds to increase diversity, equity, and inclusion within the group.

I have received my undergraduate and postgraduate degree in Applied Chemistry and Chemical Engineering, while Ph.D. in Chemical and Biological Engineering. In my Ph.D., I have worked on solving fundamental problems associated to electrochemistry using computational simulations. My diverse educational background allows me to develop expertise different major areas such as Chemical Engineering, Electrochemistry, Classical or Statistical Mechanics, Material Science and Chemistry. I am also qualified to teach theoretical chemistry, condensed matter or a course related to computational chemistry. During my Ph.D. and now in Stanford, I became an expert in catalysis and surface science and also in more specialized chemical engineering curriculum (kinetics, thermodynamics, transport). Overall, I feel qualified to teach general level undergraduate and graduate courses at the departments of physics, chemistry, and chemical engineering and to participate in a campus-wide, interdisciplinary science programs. In an ideal situation, I would create new course on the subject of "Heterogeneous catalysis and chemical bonding on surfaces" or a specialized course on “computational methods for electronic structure of materials”.

Figure 1 Design principle of highly active and durable heterogeneous catalysts for electrochemical energy conversion reaction.