If successful: Produce molecular hydrogen directly from the Sun and the seawater, thus mitigating contemporary energy and environmental challenges

List of Publications:

• Xingyun Li, Liangping Xiao, Ling Zhou, Qingchi Xu, Jian Weng, Jun Xu*, Bin Liu.* Adaptive Bifunctional Electrocatalyst of Amorphous CoFe Oxide @2D Black Phosphorus for Overall Water Splitting. Angew.Chem. Int. Ed. 2020, 59,21106. https://doi.org/10.1002/anie.202008514.

Brief description: In this work, by growing amorphous multi-transition-metal (cobalt and iron) oxide on two-dimensional (2D) black phosphorus (BP), we develop a bifunctional electrocatalyst (CoFeO@BP), which is able to efficiently catalyze both HER and OER.

• Xuning Li , Linghui Liu , Xinyi Ren , Jiajian Gao , Yanqiang Huang*, Bin Liu.* Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion. Science Advances 23 Sep 2020: Vol. 6, no. 39, eabb6833. https://advances.sciencemag.org/content/6/39/eabb6833/tab-article-info.

Brief description: In this review, we focus on the recently developed strategies of single atom catalyst (SAC) synthesis, with attention on the microenvironment modulation of single-atom active sites of SACs. Experimental and computational advances in understanding such microenvironment in association to the catalytic activity and mechanisms are summarized and exemplified in the electrochemical applications, including the water electrolysis and O2/CO2/N2 reduction reactions.

• Qilun Wang , Cong-Qiao Xu*, Wei Liu, Sung-Fu Hung, Hong Bin Yang*, Jiajian Gao , Weizheng Cai, Hao Ming Chen, Jun Li & Bin Liu.* Coordination engineering of iridium nanocluster bifunctional electrocatalyst for highly efficient and pH-universal overall water splitting. Nature Communications volume 11, Article number: 4246 (2020).    https://www.nature.com/articles/s41467-020-18064-w.pdf.

Brief description: In this work, we report uniformly dispersed iridium nanoclusters embedded on nitrogen and sulfur co-doped graphene as an efficient and robust electrocatalyst for both HER and OER at all pH conditions.

• Jiajian Gao, Xiang Huang, Weizheng Cai, Qilun Wang, Chunmiao Jia, and Bin Liu.* Rational Design of an Iridium–Tungsten Composite with an Iridium-Rich Surface for Acidic Water Oxidation. ACS Appl. Mater. Interfaces 2020, 12, 23, 25991. https://pubs.acs.org/doi/10.1021/acsami.0c05906.

Brief description: In this work, we design iridium–tungsten composites with a metallic tungsten-rich core and an iridium-rich surface by the sol–gel method followed by hydrogen reduction. The thus obtained iridium–tungsten catalyst shows much higher intrinsic water oxidation activity (100 mA/mgIr at an overpotential of 290 mV) and stability (100 h at 10 mA/cm2geom) together with reduced iridium content (33 wt % only) as compared with pure iridium oxide.

• Weizheng Cai, Rong Chen, Hongbin Yang, Hua Bing Tao, Hsin-Yi Wang, Jiajian Gao, Wei Liu, Song Liu, Sung-Fu Hung, Bin Liu.* Amorphous versus Crystalline in Water Oxidation Catalysis: A Case Study of NiFe Alloy. Nano Lett. 2020, 20, 6, 4278. https://doi.org/10.1021/acs.nanolett.0c00840 .

Brief description: Catalytic water splitting driven by renewable electricity offers a promising strategy to produce molecular hydrogen, but its efficiency is severely restricted by the sluggish kinetics of the anodic water oxidation reaction. Amorphous catalysts are reported to show better activities of water oxidation than their crystalline counterparts, but little is known about the underlying origin, which retards the development of high-performance amorphous oxygen evolution reaction catalysts. Herein, on the basis of cyclic voltammetry, electrochemical impedance spectroscopy, isotope labeling, and in situ X-ray absorption spectroscopy studies, we demonstrate that an amorphous catalyst can be electrochemically activated to expose active sites in the bulk thanks to the short-range order of the amorphous structure, which greatly increases the number of active sites and thus improves the electrocatalytic activity of the amorphous catalyst in water oxidation.

If successful: Reduce anthropogenic CO2emission,minimize waste disposal and produce value-added products.

If successful: A simple and scalable fabrication method for generating enhanced molecular sieving and high through-put membranes to accelerate the technology translation.

List of Publications:

• Ayesha Raza, Mohammad Askari, Can Zeng Liang, Na Peng, Sarah Farrukh, Arshad Hussain, Tai-Shung Chung. * Advanced multiple-layer composite CTA/CDA hollow fiber membranes for CO2 separation. Journal of Membrane Science, 625, 1 May 2021, 119124.    https://www.sciencedirect.com/science/article/abs/pii/S0376738821000776.

Brief description: In this work, novel hollow fiber composite membranes were prepared from cellulose triacetate (CTA)/cellulose diacetate (CDA) blends for efficient CO2/CH4 separation. The optimized dual-layer hollow fiber membrane samples achieved CO2 permeance of 45 GPU and ideal CO2/CH4 selectivity of 30.3 which are attractive separation metrics for practical CO¬2 capture applications.

• Ji Wu, Susilo Japip, Tai-Shung Chung.* Infiltrating molecular gatekeepers with coexisting molecular solubility and 3D-intrinsic porosity into a microporous polymer scaffold for gas separation. J. Mater. Chem. A, 2020,8, 6196.        https://pubs.rsc.org/en/content/articlelanding/2020/ta/c9ta12028a/unauth#!divAbstract.

Brief description: We demonstrated a facile post-fabrication infiltration method that allowed size-sieving cavitands to be incorporated into prefabricated dense polymer membranes. The proof-of-concept 4-sulfocalix[4]arene with a ~3.0Å cavity opening was successfully infiltrated, on a molecularly homogeneous basis, into amidoxime-functionalized PIM-1 (AOPIM-1) membranes to serve as size-sieving gatekeepers against gas transport. H2/N2, H2/CH4, H2/CO2 and CO2/CH4 separation performances were all tremendously enhanced and comparable with state-of-the-art molecular-sieving membranes.

• J. Wu, C.Z. Liang, A. Naderi, T.S. Chung. Tunable supramolecular cavities molecularly homogenized in polymer membranes for ultra-efficient precombustion CO2 capture, Adv. Mater. 34 (2022) 2105156. https://onlinelibrary.wiley.com/doi/epdf/10.1002/adma.202105156

Brief description: Processable molecular-sieving membranes are important materials for realizing energy-efficient precombustion CO2 capture during industrial-scale hydrogen production. However, the promising design of mixed matrix membranes (MMMs) that aims to integrate the molecular-sieving properties of nanoporous architectures with industrial processable polymers still faces performance and fabrication issues due to the formation of segregated nanofiller domains in their polymer matrices. Here, an unconventional nanocomposite membrane design is proposed using soluble organic macrocyclic cavitands (OMCs) with tunable open cavity sizes that not only mitigate the formation the discrete nanofiller phases but also deliver distinct molecular-sieving separations.

• J. Wu, T.S. Chung. Supramolecular polymer network membranes with molecular-sieving nanocavities for efficient pre-combustion CO2 capture, Small Methods 6 (2022) 2101288. https://onlinelibrary.wiley.com/doi/epdf/10.1002/smtd.202101288

If successful: Improve the wet CO2 uptake and thus reduce the energy penalty beyond the present level of 25 – 40%.

List of Publications:

• Kang, C. J., Zhang, Z. Q., Wee, V., Usadi, A. K., Calabro, D. C.; Baugh, L. S., Wang, S., Wang, Y. X., Zhao, D.* Interlayer shifting in two-dimensional covalent organic frameworks. J. Am. Chem. Soc. 2020, 142, 12995. (Supplementary Cover).    https://pubs.acs.org/doi/10.1021/jacs.0c03691.

Brief Description: Covalent organic frameworks (COFs) are a family of crystalline porous polymers with high surface areas and tunable functionalities. For the first time, this work reveals the interlayer shifting phenomenon in 2D COFs in a solvated state, suggesting new opportunities for the applications of COFs in liquid-phase chemical separations, molecular sensing, and heterogeneous catalysis.

• Peh, S. B., Zhao, D.* Tying amines down for stable CO2 capture. Science 2020, 369, 372.    https://science.sciencemag.org/content/369/6502/372.

Brief description: This perspective paper summarizes and analyzes a new amine-appended MOF material, which possesses high CO2/H2O and CO2/N2 selectivity. This combination of attributes is promising for applications in water-containing CO2 capture scenarios, such as post combustion capture from NGCC plants.

• A metal-organic framework (MOF)-based temperature swing adsorption cycle for postcombustion CO2 capture from wet flue gas. Chem. Eng. Sci. 2022, 250, 117399. https://www.sciencedirect.com/science/article/pii/S0009250921009647?via%3Dihub

Brief description:

Competitive adsorption or structural degradation by water has been found to be a major concern in the viability of solid CO₂ sorbents. In this work, we report a simulation-based feasibility study of a single-stage temperature swing adsorption (TSA) process operated on a metal–organic framework (MOF) adsorbent, UTSA-16, for CO₂ capture and concentration from a wet flue gas without pre-drying or a desiccant pre-layer. Two TSA cycles have been synthesized meeting 95% purity-90% recovery targets set by the U.S. Department of Energy for postcombustion carbon capture.

If successful: Enhance the energy efficiency and thus, reduce carbon emissions from refining and chemical sectors

List of Publications:

• Homa Hamedi, Iftekhar A. Karimi,* Truls Gundersen.* Simulation-based approach for integrating work within heat exchange networks for ambient processes. Energy Conversion and Management 203 (2020) 112276.        https://www.sciencedirect.com/science/article/abs/pii/S0196890419312828.

Brief description: A simulation-based methodology is developed for work-integrated heat exchange network-synthesis which needs no correlations or simplifying assumptions. For this, a generalized superstructure is developed, which accommodates liquid and vapor phase and reduces the search region for network synthesis. Particle-swarm optimization approach is used for solving non-convex optimization problem.