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The research programs in Zhang Group are focused on the development of novel organic functional materials and their composites, aimed at addressing key challenges in environmental and energy applications. Central to our research is the exploration of innovative synthetic methodologies, particularly in dynamic covalent chemistry (DCvC), which enable efficient, high-yield synthesis and pave the way toward more sustainable and high-performance materials. 

DYNAMIC COVALET CHEMICAL REACTIONS

Our group has been pioneering the development and application of dynamic covalent chemistry (DCvC)--including alkyne metathesis with related catalyst development, dynamic imine chemistry, dynamic nucleophilic aromatic substitution (SNAr), and dynamic spiroborate chemistry. These reactions are powerful tools not only for constructing well-defined ordered molecular and polymeric architectures, but also for synthesizing functional materials with adaptive properties and controlled reversibility. The development of new dynamic covalent chemical reactions has become critical, not only to enhance our synthetic capabilities but also to expand the range of materials accessible through controlled assembly. By continuously refining the dynamic reactions and their catalysts, we aim to push the boundaries of DCvC, offering a robust foundation for the next generation of functional materials. 

SHAPE-PERSISTENT 2D AND 3D MOLECULAR ARCHITECTURES

Shape-persistent molecular architectures in both two and three dimensions are a key component in our research, particularly for applications in molecular separation and the controlled growth of nanoparticles (NPs). Utilizing DCvC, our group has achieved high yields of 2D macrocycles and 3D cages by leveraging the thermodynamic favorability of specific target products. This approach, which contrasts with conventional kinetic-controlled methods, allows us to construct rigid, well-defined structures from simple building blocks. We envision that these structures open new possibilities in nanotechnology, where precision and predictability are key in applications ranging from catalysis to nanocomposite formation.

STRUCTURALLY ORDERED POLYMERIC ARCHITECTURES 

Our research in structurally ordered polymers includes significant advancements in 2D or 3D covalent organic frameworks (COFs) and ionic covalent organic frameworks (ICOFs). These frameworks, noted for their chemical and thermal stability, present vast potential for applications in gas separation, catalysis, ion transportation and beyond. Our efforts also extend to helical covalent polymers, where we investigate their unique chiral properties and stability under dynamic conditions. By focusing on well-ordered polymeric architectures, we aim to contribute to the development of solution-processable and structurally ordered materials, overcoming current limitations in the field of porous polymers and offering enhanced functionalities. 

DYNAMIC NETWORK POLYMERS

We have also been working on the development of dynamic covalent adaptable networks (CANs) to create polymers that exhibit malleability, rehealability, and closed-loop recyclability, highlighting their great potential for sustainable applications. Our recent work has led to the synthesis of self-healing and easily reprocessable network polymers, making them versatile for diverse applications and enabling efficient recycling processes. By integrating dynamic covalent bonds into the polymer backbone and crosslinks, we can achieve materials that retain robust mechanical properties while allowing recyclability—a critical advancement for the sustainable material field.

• Lei, Z.; Wang, Z.; Jiang, H.; Cahn, J. R.; Chen, H.; Huang, S.; Jin, Y.; Wang, X.; Yu, K.; Zhang, W.* “Dual-factor Controlled Dynamic Precursors Enable On-demand Thermoset Degradation and Recycling” Adv. Mater. 2024, 36, in press. 
• Kim, Y.*; Li, C.; Huang, J.; Yuan, Y.; Tian, Y.; Zhang, W.* “Ionic Covalent Organic Framework Solid-State Electrolytes” Adv. Mater. 2024, 36, 2407761.
• Hu, Y.; Sengupta, B.; Long, H.; Wayment, L. J.; Ciora, R.; Jin, Y.; Wu, J.; Lei, Z.; Friedman, K.; Chen, H.; Yu, M.*; Zhang, W.* “Molecular Recognition with Resolution below 0.2 Å via Thermo-regulatory Oscillations in Covalent Organic Frameworks”, Science 2024, 384, 1441-1447. 
• Wayment, L. J.; Huang, S.; Chen, H.; Lei, Z.; Ley, A.; Lee, S.-H.; Zhang, W.* “Ionic Covalent Organic Frameworks Consisting of Tetraborate Nodes and Flexible Linkers” Angew. Chem. Int. Ed. 2024, 63, e202410816. 
• Huang, S.; Teat, S. J.; Wayment, L. J.; Settineri, N. S.; Chen, H.; Lei, Z.; Zhang, W.* “Single-Crystal Cage Framework with High Selectivity and Reversibility in Fullerene Binding” Angew. Chem. Int. Ed. 2024, 63, e202409432. 
• Lei, Z.; Chen, H.; Huang, S.; Wayment, L. J.; Xu, Q.; Zhang, W.* “New Advances in Covalent Network Polymers via Dynamic Covalent Chemistry” Chem. Rev. 2024, 124, 7829-7906. (Front Cover, invited). 
• Wayment, L. J.; Teat, S. J.; Huang, S.; Chen, H.; Zhang, W.* “Dynamic Entwined Topology in Helical Covalent Polymer Dictated by Competing Supramolecular Interactions” Angew. Chem. Int. Ed. 2024, 63, e202403599.
• Xu, Q.; Wang, X.; Huang, S.; Hu, Y.; Teat, S. J.; Settineri, N. S.; Chen, H.; Wayment, L. J.; Jin, Y.; Sharma, S.; Zhang, W.* “Dynamic Covalent Self-sorting in Molecular and Polymeric Architectures Enabled by Spiroborate Bond Exchange” Angew. Chem. Int. Ed. 2023, 62, e2023042. 
• Chen, H.; Hu, Y.; Luo, C.; Lei, Z.; Huang, S.; Jin, Y.; Yu, K.; Zhang, W.* “Spiroborate-linked Ionic Covalent Adaptable Networks with Rapid-reprocessability and Closed-loop Recyclability” J. Am. Chem. Soc. 2023, 145, 9112-9117.
• Huang, S.; Choi, J. Y.; Xu, Q. ; Jin, Y. ; Park, J.* ; Zhang, W.* “Carbazolylene-Ethynylene Macrocycle based Conductive Covalent Organic Frameworks” Angew. Chem. Int. Ed. 2023, 62, e2023035.
• Wayment, L. J.; Wang, X.; Huang, S.; McCoy M. S.; Chen, H.; Hu, Y.; Jin, Y.; Sharma, S.; Zhang, W.* “3D Covalent Organic Framework as a Metastable Intermediate in the Formation of a Double-stranded Helical Covalent Polymer” J. Am. Chem. Soc. 2023, 145, 15547–15552.
• Lei, Z.; Wayment, L.; Cahn, J. R.; Chen, H.; Huang, S.; Jin, Y.; Zhang, W.* “Cyanurate-linked Covalent Organic Frameworks Enabled by Dynamic Nucleophilic Aromatic Substitution” J. Am. Chem. Soc., 2022, 144, 39, 17737–17742.
• Lei, Z.; Chen, H.; Luo, C.; Rong, Y.; Hu, Y.; Jin, Y.; Long, R.; Yu, K.; Zhang, W.* “Recyclable and Malleable Thermosets Enabled by Activating Dormant Dynamic Linkages” Nat. Chem. 2022, 14, 1399-1404.
• Hu, Y.; Teat, S. J.; Gong, W.; Zhou, Z.; Jin, Y.; Chen, H.; Wu, J.; Cui, Y.; Jiang, T.; Cheng, X.; Zhang, W.* “Single-Crystal Mechanically Entwined Helical Covalent Polymer” Nat. Chem. 2021, 13, 660-665.
• Ge, Y.; Huang, S.; Hu, Y.; Zhang, L.; He, L.; Krajewski, S.; Ortiz, M.; Jin, Y.; Zhang, W.* “Highly Active Multidentate Molybdenum-carbyne Complexes Catalyzing Alkyne Metathesis under Open Air Condition” Nat. Commun. 2021, 12, 1136.
• Jin, Y.; Wang, Q.; Taynton, P.; Zhang, W. Dynamic Covalent Chemistry Approach Towards 2-D Macrocycles, 3-D Molecular Cages, and Polymers. Acc. Chem. Res. 2014, 47, 1575-1586.
• Heat or Water Driven Malleability in a Highly-Recyclable Covalent Network Polymer. Taynton, P.; Yu, K.; Shoemaker, R.; Jin, Y.; Qi, H. J.; Zhang, W. Adv. Mater. 2014, 26, 3938-3942.
• Template Synthesis of Gold Nanoparticles with an Organic Molecular Cage. McCaffrey, R.; Long, H.; Jin, Y.; Sanders, A.; Park, W.; Zhang, W. J. Am. Chem. Soc. 2014, 136, 1782-1785.
• Recent Advances in Dynamic Covalent Chemistry. Jin, Y.; Yu, C.; Denman, R. J.; Zhang, W. Chem. Soc. Rev. 2013, 42, 6634-6654.
• Solution Processable Polydiacetylenes (PDAs) through Acyclic Enediyne Metathesis Polymerization. Hu, K.; Yang, H.; Zhang, W.; Qin, Y. Chem. Sci. 2013, 4, 3649-3653.
• Imine-linked Porous Polymer Frameworks with High Small Gas (H2, CO2, CH4, C2H2) Uptake and CO2/N2 Selectivity. Zhu, Y.; Long, H.; Zhang, W. Chem. Mater. 2013, 25, 1630-1635.
• Highly Active Multidentate Alkyne Metathesis Catalysts: Ligand-activity Relationship and Their Applications in Efficient Synthesis of Porphyrin-based Aryleneethynylene Polymers. Jyothish, K.; Wang, Q.; Zhang, W. Adv. Synth. Catal. 2012, 354, 2073-2078.
• Microwave-Assisted Syntheses of Highly CO2-Selective Organic Cage Frameworks (OCFs). Jin, Y.; Voss, B. A.; McCaffrey, R.; Baggett, C. T.; Noble, R. D.; Zhang, W. Chem. Sci. 2012, 3, 874-877.
• A Highly C70-Selective Shape-Persistent Rectangular Prism Constructed Through One-Step Alkyne Metathesis. Zhang, C.-X.; Wang, Q.; Long, H.; Zhang, W. J. Am. Chem. Soc. 2011, 133, 20995-21001.
• Towards Highly Active and Robust Alkyne Metathesis Catalysts: Recent Developments in Catalyst Design. Jyothish, K.; Zhang, W. Angew. Chem. Int. Ed. 2011, 50, 8478-8480.
• Highly CO2-Selective Organic Molecular Cages: What Determines the CO2 Selectivity. Jin, Y.; Voss, B. A.; Jin, A.; Long, H.; Noble, R. D.; Zhang, W. J. Am. Chem. Soc. 2011, 133, 6650-6658.
• Introducing Podand Motif to Alkyne Metathesis Catalyst Design: A Highly Active Multidentate Mo(VI) Catalyst Resisting Alkyne Polymerization. Jyothish, K.; Zhang, W. Angew. Chem. Int. Ed. 2011, 50, 3435-3438.
• Shape-Persistent Arylenevinylene Macrocycles (AVMs) Prepared via Acyclic Diene Metathesis Macrocyclization (ADMAC). Jin, Y.; Zhang, A.; Huang, Y.; Zhang, W. Chem. Commun. 2010, 46, 8258-8260.
• A Shape-Persistent Organic Molecular Cage with High Selectivity in Adsorption of CO2 over N2. Jin, Y.; Voss, B.; Noble, R. D.; Zhang, W. Angew. Chem. Int. Ed. 2010, 49, 6348-6351.
• Modular Functionalization of Carbon Nanotubes and Fullerenes. Zhang, W.; Sprafke, J. K.; Ma, M.; Tsui, E. Y.; Sydlik, S. A; Rutledge, G. C; Swager, T. M. J. Am. Chem. Soc. 2009, 131, 8446.
• Functionalization of Single-Walled Carbon Nanotubes and Fullerenes via a Dimethyl Acetylenedicarboxylate-4-Dimethylaminopyridine Zwitterion Approach. Zhang, W.; Swager, T. M. J. Am. Chem. Soc. 2007, 129, 7714.
• Shape-Persistent Macrocycles: Structures and Synthetic Approaches from Arylene and Ethynylene Building Blocks. Zhang, W.; Moore, J. S. Angew. Chem. Int. Ed. 2006, 45, 4416.
• Reaction Pathways Leading to Arylene Ethynylene Macrocycles via Alkyne Metathesis. Zhang, W.; Moore, J. S. J. Am. Chem. Soc. 2005, 127, 11863.
• Arylene Ethynylene Macrocycles Prepared by Precipitation-Driven Alkyne Metathesis. Zhang, W.; Moore, J. S. J. Am. Chem. Soc. 2004, 126, 12796.
• Highly Active Trialkoxymolybdenum(VI) Alkylidyne Catalysts Synthesized by a Reductive Recycle Strategy. Zhang, W.; Kraft, S.; Moore, J. S. J. Am. Chem. Soc. 2004, 126, 329.