Creating Nanoknot‐Like Domains for Robust Artificial Spider Silk Toward High Twistocaloric Performance

J Jiatian Li (State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China) G Guangkai Mei (State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Tianjin Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China) S Shaoli Fang (Alan G. MacDiarmid Nanotech Institute University of Texas at Dallas Richardson Texas USA) X Xiao Liu S Songen Liu (State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China) Y Yasi Liu (State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Tianjin Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China) Z Zhaoyu Yang X Xuanliang Han (Department of Science China Pharmaceutical University Nanjing China) M Meilin Wang Y Yicheng Xiao (State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China) W Wang Chang W Wenjin Guo W Weiqiang Zhao (1Shenzhen University General Hospital, Shenzhen, China) G Guanghao Zhang Z Ziqian Zhang C Chao Li M Mengmeng Zhang (Breast Center) J Jie Bai (State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering & Institute of Artificial Intelligence & Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM)) X Xiang Zhou R Ray H. Baughman (Alan G. MacDiarmid NanoTech Institute, University of Texas at Dallas) Z Zunfeng Liu (State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Tianjin Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China)

Abstract

ABSTRACT High‐efficiency refrigeration materials with long cycle lifetimes are essential for reducing energy consumption in conventional cooling systems. Twistocaloric cooling, which harnesses nonlinear torsional stress, offers a promising pathway to enhanced cooling efficiency. However, a general design strategy for polymer‐based twistocaloric materials that combine high efficiency and long cycle life remains elusive. Here, we report spider silk‐inspired polybiurea elastomer fibers that exhibit exceptional mechanical properties and twistocaloric cooling performance. The material's architecture features nanoknot‐like domains formed via multiple hydrogen bonds and π – π interactions in the hard segments, which knot together the soft segments to provide high mechanical stability and substantial entropy changes. The polybiurea fibers with nanoknot‐like domains achieved an extraordinary combination of breaking strength of 316.5 MPa and toughness of 523.4 MJ m −3 . This engineered deformable knotted structure enables a maximum cooling temperature drop of −17.1 K (by twisting and stretching), a maximum Carnot efficiency of 89.7%, and operational durability up to 120 000 mechanical fatigue life cycles. We further demonstrate two out‐of‐phase operated twistocaloric devices designed to recover input mechanical energy, thereby enhancing overall system efficiency. This work presents a robust materials strategy for advancing high‐performance polymeric refrigeration materials and systems.

Article Details

Volume / Issue Vol. 38, Issue 21
Published April 01, 2026
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (21)

J

Jiatian Li

State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China

G

Guangkai Mei

State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Tianjin Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China

S

Shaoli Fang

Alan G. MacDiarmid Nanotech Institute University of Texas at Dallas Richardson Texas USA

X

Xiao Liu

S

Songen Liu

State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China

Y

Yasi Liu

State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Tianjin Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China

Z

Zhaoyu Yang

X

Xuanliang Han

Department of Science China Pharmaceutical University Nanjing China

M

Meilin Wang

Y

Yicheng Xiao

State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China

W

Wang Chang

W

Wenjin Guo

W

Weiqiang Zhao

1Shenzhen University General Hospital, Shenzhen, China

G

Guanghao Zhang

Z

Ziqian Zhang

C

Chao Li

M

Mengmeng Zhang

Breast Center

J

Jie Bai

State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering & Institute of Artificial Intelligence & Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM)

X

Xiang Zhou

R

Ray H. Baughman

Alan G. MacDiarmid NanoTech Institute, University of Texas at Dallas

Z

Zunfeng Liu

State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Functional Polymer Materials Tianjin Key Laboratory of Functional Polymer Materials Frontiers Science Center for New Organic Matter College of Chemistry Nankai University Tianjin China