4.8 Article

Intrinsic Role of Molecular Architectonics in Enhancing the Catalytic Activity of Lead in Glucose Hydrolysis

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 12, Issue 12, Pages 14057-14063

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c01803

Keywords

molecular architectonics; self-assembly; glucose hydrolysis; metal-supported catalyst; second coordination sphere

Funding

  1. JNCASR, SwarnaJayanti Fellowship [DST/SJF/CSA-02/2015-2016]
  2. BRICS Multilateral R&D Projects Grant [DST/IMRCD/BRIC/PilotCAll2/EPNAPT/2018(G)]
  3. Department of Science and Technology (DST) Grant Govt. of India
  4. Sheikh Saqr Laboratory (SSL), ICMS-JNCASR

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Lewis acidity plays a key role in the catalytic activity of lead ion (Pb-II) in the hydrolysis of glucose in solution under harsh synthetic conditions. We report a number of structurally similar D-gluconamide amphiphiles as functional organic ligands with active an -NH center capable of coordinating Pb-II (viz., Pb-II-N-C) in basic condition to enhance the catalytic efficiency through the scheme of molecular architectonics. Amphiphiles with different hydrophobic unit form assembly-architectures with a varying second coordination sphere around the active metal ion center. As a result, the active Pb-II center in each architecture exhibits substantially different efficiency toward catalyzing the glucose hydrolysis under ambient temperature. The catalytic performance of the dynamic and reversible gluconamide-Pb-II assembly-architectures are highly dependent on their chemical environments in solution. Further, the active Pb-II center of gluconamide-Pb-II complex in the assembly architecture and dispersed states exhibits distinct outcomes with the former being a superior catalyst than the latter as well as Pb-II alone. The current study demonstrates the potential of molecular architectonics that relies on the hydrophobic units of designer functional amphiphiles to enrich surface electron density with enhanced a-donation ability through space which substantially improves the catalytic efficiency of Pb-II toward glucose hydrolysis at ambient temperature.

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