Nanobiomineralization of Carbon Dioxide by Molecularly Engineered Metal-Histidine Complex Nanozymes

被引:7
作者
Nilouyal, Somaye [1 ,2 ]
Karahan, H. Enis [1 ,2 ,3 ]
Ng, Elvis Wang Hei [4 ]
Yamaguchi, Daisuke [1 ,2 ]
Ito, Masateru M. M. [1 ,2 ]
Qin, Detao [1 ,2 ]
Hirao, Hajime [4 ]
Sivaniah, Easan [1 ,2 ]
Ghalei, Behnam [1 ,2 ]
机构
[1] Kyoto Univ, Inst Integrated Cell Mat Sci iCeMS, Kyoto 6068501, Japan
[2] Kyoto Univ, Grad Sch Engn, Dept Mol Engn, Kyoto 6158510, Japan
[3] Istanbul Tech Univ, Synthet Fuels & Chem Technol Ctr ITU SENTEK, TR-34469 Istanbul, Turkiye
[4] Chinese Univ Hong Kong, Warshel Inst Computat Biol, Sch Life & Hlth Sci, Sch Med, Shenzhen 518172, Guangdong, Peoples R China
关键词
CO2; HYDRATION; ANHYDRASE; CAPTURE; TRANSITION;
D O I
10.1021/acs.chemmater.2c03169
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Next-generation carbon capture, utilization, and storage (CCUS) technologies will be indispensable elements of global decarbonization efforts. In this context, permanent and rapid sequestration of carbon dioxide (CO2) at high capacities will impact their utility broadly. CO2 mineralization into solid inorganic carbonates is an appealing CCUS approach, which requires fast CO2 hydration for effective implementation. The carbonic anhydrases (CAs) have, thus, gained considerable attention as rate promoters for CO2 hydration. Nevertheless, the poor stability and high cost of CAs limit their practical application prospects. Here, we demonstrate that the molecular size control of histidine-based bolaamphiphiles (HisBolas) is a viable strategy for forming robust nanoarchitectures with unusual CA-like catalytic activity. HisBola molecules self-assemble into nanoparticles (similar to 40 nm) that fuse into globules in water, and the metal coordination of these supramolecular nanoassemblies results in nanozymes. The developed bioinspired nanozymes boost the CO2 hydration kinetics, thus efficiently catalyzing the mineralization process. Systematically studying the alkyl chain length of HisBolas (HisBola5, 7, and 10), we optimized the catalytic activity of the nanozymes. The nanozyme with the optimum structure, zinc-coordinated HisBola5, showed the highest esterase activity [kcat/Km of similar to 33.44 M-1 center dot s-1 and Michaelis constant (Km) of similar to 0.29 mM] and CO2 hydration kinetics (kcat.hyd/Km.hydof similar to 30,300 M-1 center dot s-1 and Km.hyd of similar to 14 mM) among all metal-coordinated HisBolas screened. Overall, low-molecular-weight HisBolas offer a promising platform for designing metal-coordinated nanozymes with high catalytic activity, outstanding thermal stability, and rapid catalytic CO2 hydration ability for CO2 mineralization. We argue that the alkyl unit-controlled performance manipulation of produced nanozymes offers a new path for engineering supramolecular CA mimics, which share a common trait with proteinaceous enzymes, that is, the supporting role of noncatalytic units in catalytic activity.
引用
收藏
页码:1610 / 1623
页数:14
相关论文
共 72 条
[1]   Directed evolution of an ultrastable carbonic anhydrase for highly efficient carbon capture from flue gas [J].
Alvizo, Oscar ;
Nguyen, Luan J. ;
Savile, Christopher K. ;
Bresson, Jamie A. ;
Lakhapatri, Satish L. ;
Solis, Earl O. P. ;
Fox, Richard J. ;
Broering, James M. ;
Benoit, Michael R. ;
Zimmerman, Sabrina A. ;
Novick, Scott J. ;
Liang, Jack ;
Lalonde, James J. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2014, 111 (46) :16436-16441
[2]   Carbonic Anhydrases: Versatile and Useful Biocatalysts in Chemistry and Biochemistry [J].
Angeli, Andrea ;
Carta, Fabrizio ;
Supuran, Claudiu T. .
CATALYSTS, 2020, 10 (09) :1-11
[3]   GFN2-xTB-An Accurate and Broadly Parametrized Self-Consistent Tight-Binding Quantum Chemical Method with Multipole Electrostatics and Density-Dependent Dispersion Contributions [J].
Bannwarth, Christoph ;
Ehlert, Sebastian ;
Grimme, Stefan .
JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 2019, 15 (03) :1652-1671
[4]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[5]   Self-Assembly of Amphiphilic Dipeptide with Homo- and Heterochiral Centers and Their Application in Asymmetric Aldol Reaction [J].
Bhowmick, Sudipto ;
Zhang, Li ;
Ouyang, Guanghui ;
Liu, Minghua .
ACS OMEGA, 2018, 3 (07) :8329-8336
[6]   Bioinspired Metal-Organic Framework for Trace CO2 Capture [J].
Bien, Caitlin E. ;
Chen, Kai K. ;
Chien, Szu-Chia ;
Reiner, Benjamin R. ;
Lin, Li-Chiang ;
Wade, Casey R. ;
Ho, W. S. Winston .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (40) :12662-12666
[7]   Self-assembly of aramid amphiphiles into ultra-stable nanoribbons and aligned nanoribbon threads [J].
Christoff-Tempesta, Ty ;
Cho, Yukio ;
Kim, Dae-Yoon ;
Geri, Michela ;
Lamour, Guillaume ;
Lew, Andrew J. ;
Zuo, Xiaobing ;
Lindemann, William R. ;
Ortony, Julia H. .
NATURE NANOTECHNOLOGY, 2021, 16 (04) :447-+
[8]   Carbon Capture and Sequestration [J].
Chu, Steven .
SCIENCE, 2009, 325 (5948) :1599-1599
[9]   Investigation of surfactant conformation and order at the liquid-liquid interface by total internal reflection sum-frequency vibrational spectroscopy [J].
Conboy, JC ;
Messmer, MC ;
Richmond, GL .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (18) :7617-7622
[10]   Tetrahedral vs octahedral zinc complexes with ligands of biological interest: A DFT/CDM study [J].
Dudev, T ;
Lim, C .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (45) :11146-11153