(4cq) Capture and Conversion of CO2 – Towards CO2 Recycling

Our current global fossil fuel-based energy economy produces significant environmental problems (e.g., climate change, SO_x, NO_x emissions, etc.) and energy injustice – whereby our energy systems unequally distribute benefits, access, and burden across different communities. Environmental concerns associated with CO₂ and CH₄ emissions and economic forces that have reduced the costs of renewable energy are pushing towards the stepwise decarbonization of our economy. The coming transition should be approached in a holistic way considering not only environmental and economic factors, but also social factors. Ideally, we will move towards a more just energy system, while minimizing the creation of new avenues of injustices. To this end, my research program centers around developing engineering solutions for CO₂ capture, use and recycle, with an eye towards both short term and long-term goals. In the short term, engineering solutions must be robust, economic, and practical. In the longer term, we can envision a circular CO₂ economy that uses CO₂ as a carbon building block and sustainably and equitably cycles carbon from the atmosphere or other wastes into fuels and products. Overall, my group will tackle challenges at the energy-sustainability-community intersection with a foundation rooted in basic science principles and an eye towards engineering innovation. Critically, CO₂ management plays a major role in achieving this overall goal.

In my Ph.D. research with Prof. Eranda Nikolla at Wayne State University, I tackled the design of electrocatalyst to facilitate electrochemical reactions happening in the electrodes of Reversible Solid Oxide Cells (RSOCs). These devices are a promising class of electrochemical technologies that operate at high temperatures (T > 700°C) and can interchangeably convert electricity into chemical energy and back to electricity. They have potential to become an essential part of processes that transform CO₂ and H₂O into hydrocarbons – a key part of the carbon recycling system.

Correspondingly, my PhD thesis focused on the rational design of electrocatalysts and on obtaining fundamental insights into the electrode design that can enable better energy efficiency in these cells – minimizing overpotential losses and lowering the operating temperatures. I combined controlled synthesis, advanced characterization, density functional calculations and catalytic evaluation as effective ways for developing the fundamental, molecular level knowledge required to guide the design of efficient electrocatalysts for CO₂ reduction and oxygen electrocatalysis.^1-5 This knowledge opened up possibilities for the enhancement of surface reactivity that can be achieved via nanoengineering of mixed metal oxides materials for RSOCs.^{6, 7}

In my postdoctoral work at Georgia Tech in the lab of Prof. Christopher Jones, my focus has been on the direct air capture (DAC) of CO₂ using solid sorbents – where chemisorbent amines are supported in porous solids. My work has explored the temporal change occurring in sorbents during DAC processes, aiming to identify fundamental mechanisms and elucidating key parameters that impact degradation of sorbent materials. In this research I have developed expertise in synthesis and characterization of hybrid polymeric and microporous materials for CO₂ capture. I combined several complementary characterization techniques, including CO₂ sorption kinetics, elemental analysis, and in situ IR spectroscopy to obtain an understanding of the sorbent degradation process. These findings provide important insights into the relevant parameters that impact the effective design of DAC sorbents & processes for implementation in different climates.^{8, 9}

As a future faculty member, I plan to use my repertoire in electro/heterogeneous catalysis, material design and process engineering to target issues related to air pollution control. I will accomplish this via the development of adsorption and reaction processes for CO₂ capture and utilization – cornerstone technologies needed to shift our current carbon economy from a linear model to a circular model.

Teaching Interests

My personal ambitions in contributing to energy security, environmental sustainability as well as social advances have their foundation rooted in research and education. I believe in education as a major driving force for social mobility and with these values I plan to use research and teaching as tools to positively impact and enrich the lives of my students. During my PhD studies, I combined my technical work with mentoring and motivational activities through involvement in inclusion and mentorship projects. One example is the GO-GIRLs program at Wayne State University, a program designed to encourage Detroit-area girls to consider education and careers in STEM fields. Also, I have proudly mentored successful undergraduate students: two of which were awarded prizes in the national poster competition of the Catalysis and Reaction Engineering Division at the American Institute of Chemical Engineering (AIChE) Annual Meeting. Further, I have published scientific papers with several undergraduates, who, motivated by the experience, are now pursuing PhDs in Chemical Engineering.

As I move into my independent career, I will continue to be committed to an inclusive classroom, facilitating a diverse student population in expanding their world views while building strong technical knowledge and skills. Part of my commitment to diversity and accessibility in education includes the implementation of teaching approaches that will value different learning styles with a long-term eye on universal design. I plan to achieve this goal by promoting a supportive classroom environment, where students will be engaged via laboratory experiences, real-world inspired project work and updated scientific literature discussions to promote innovative solutions. Moreover, I would like to promote a stimulating learning environment, where students will critically reflect on traditional engineering design and its intersection with social issues, both contributing to and alleviating societal challenges. I believe that such active learning approaches will cultivate the development of a new generation of critical thinkers, who are problem-solving and compassionate engineers, scientists, and policy makers. With my multi-disciplinary training in chemical and environmental engineering, I would be able to teach engineering classes on kinetics and catalysis, thermodynamics, mass/energy balances and separations processes. I am also very interested in developing elective lectures and lab-based courses on surface science, materials science, as well as electrochemical engineering and nanotechnology, with focus on environmental remediation.

Selected Publications

^† Denotes equal contribution from both authors

1. Gu, X.-K.^†; Carneiro, J. S.^†; Samira, S.; Das, A.; Ariyasingha, N. M.; Nikolla, E., Efficient oxygen electrocatalysis by nanostructured mixed-metal oxides. Journal of the American Chemical Society 2018, 140 (26), 8128-8137.
2. Carneiro, J. S. A.; Brocca, R. A.; Lucena, M. L. R. S.; Nikolla, E., Optimizing cathode materials for intermediate-temperature solid oxide fuel cells (SOFCs): Oxygen reduction on nanostructured lanthanum nickelate oxides. Applied Catalysis B: Environmental 2017, 200, 106-113.
3. Ma, X.^†; Carneiro, J. S.^†; Gu, X.-K.^†; Qin, H.; Xin, H.; Sun, K.; Nikolla, E., Engineering complex, layered metal oxides: High-performance nickelate oxide nanostructures for oxygen exchange and reduction. ACS Catalysis 2015, 5 (7), 4013-4019.
4. Carneiro, J.; Gu, X.-K.; Tezel, E.; Nikolla, E., Electrochemical Reduction of CO2 on Metal-Based Cathode Electrocatalysts of Solid Oxide Electrolysis Cells. Industrial & Engineering Chemistry Research 2020, 59 (36), 15884-15893.
5. Gu, X.-K.; Carneiro, J. S.; Nikolla, E., First-principles study of high temperature CO2 electrolysis on transition metal electrocatalysts. Industrial & Engineering Chemistry Research 2017, 56 (21), 6155-6163.
6. Carneiro, J.; Nikolla, E., Nanoengineering of solid oxide electrochemical cell technologies: An outlook. Nano Research 2019, 12 (9), 2081-2092.
7. Carneiro, J. S.; Williams, J.; Gryko, A.; Herrera, L. P.; Nikolla, E., Embracing the Complexity of Catalytic Structures: A Viewpoint on the Synthesis of Nonstoichiometric Mixed Metal Oxides for Catalysis. ACS Catalysis: 2019.
8. Nezam, I.; Xie, J.; Golub, K. W.; Carneiro, J.; Olsen, K.; Ping, E. W.; Jones, C. W.; Sakwa-Novak, M. A., Chemical Kinetics of the Autoxidation of Poly (ethylenimine) in CO2 Sorbents. ACS Sustainable Chemistry & Engineering 2021.
9. Carneiro, J.; Jones, C. W., Important Impact of Ambient Humidity on the Oxidative Stability of Solid Amine Sorbents for Direct CO2 Capture from Air. In Preparation 2021.