Real-time monitoring of hydrophobic aggregation reveals a critical role of cooperativity in hydrophobic effect

Liguo Jiang, Siqin Cao, Peter Pak-Hang Cheung, Xiaoyan Zheng, Chris Wai Tung Leung, Qian Peng, Zhigang Shuai, Ben Zhong Tang, Shuhuai Yao () and Xuhui Huang ()
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Liguo Jiang: Institute for Advanced Study, The Hong Kong University of Science and Technology
Siqin Cao: The Hong Kong University of Science and Technology
Peter Pak-Hang Cheung: The Hong Kong University of Science and Technology
Xiaoyan Zheng: The Hong Kong University of Science and Technology
Chris Wai Tung Leung: The Hong Kong University of Science and Technology
Qian Peng: Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences
Zhigang Shuai: Tsinghua University
Ben Zhong Tang: The Hong Kong University of Science and Technology
Shuhuai Yao: HKUST-Shenzhen Research Institute
Xuhui Huang: The Hong Kong University of Science and Technology

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract The hydrophobic interaction drives nonpolar solutes to aggregate in aqueous solution, and hence plays a critical role in many fundamental processes in nature. An important property intrinsic to hydrophobic interaction is its cooperative nature, which is originated from the collective motions of water hydrogen bond networks surrounding hydrophobic solutes. This property is widely believed to enhance the formation of hydrophobic core in proteins. However, cooperativity in hydrophobic interactions has not been successfully characterized by experiments. Here, we quantify cooperativity in hydrophobic interactions by real-time monitoring the aggregation of hydrophobic solute (hexaphenylsilole, HPS) in a microfluidic mixer. We show that association of a HPS molecule to its aggregate in water occurs at sub-microsecond, and the free energy change is −5.8 to −13.6 kcal mol−1. Most strikingly, we discover that cooperativity constitutes up to 40% of this free energy. Our results provide quantitative evidence for the critical role of cooperativity in hydrophobic interactions.

Date: 2017
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DOI: 10.1038/ncomms15639

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