Silkworm cocoon-inspired and robust nanofibrous composite separator with gradient structure for lithium ion batteries.

[Display omitted] • A bioinspired nanofibrous composite separator (GPS) with concentration gradient along thickness direction was fabricated. • The GPS separator presented significantly improved mechanical strength while maintaining relatively high porosity. • Structural strengthening mechanism and lithium-ion transport ability were verified by simulation and model analysis. • Cell with the GPS separator exhibited high discharge capacity and stable cycling performance. Considering electrospun nanofiber-based membranes that generally exhibit high porosity but poor mechanical property, there is a growing need to fabricate nanofibrous separators with comprehensive performance for lithium-ion batteries (LIBs). Silkworm cocoon, a source of design inspiration from nature, comprises a multilayer structure with composition change in the thickness direction, thereby endowing the cocoon with relatively high porosity and outstanding mechanical strength. Therefore, a silkworm cocoon-like structured nanofibrous separator (GPS) is fabricated in this work by initially preparing several polyacrylonitrile (PAN) nanofibrous membranes with varied content of carboxyl styrene butadiene latex (SBR) and then laminating them in a concentration gradient sequence. Compared with the pristine PAN membrane, the GPS exhibits comparable porosity, thermal stability and electrolyte wettability due to the existence of PAN nanofibers, while the tensile strength and puncture resistance of the GPS are greatly raised by 5.5 times and 1.5 times, respectively. On account of the structure design, GPS also shows better mechanical strength than PAN/SBR separators without concentration gradient, and the strengthening mechanism has been verified by the finite element analysis. Meanwhile, such gradient structure of GPS renders the battery with desirable ion transport ability and stable cycle properties. Thus, the silkworm cocoon-like structured separator could be a promising separator candidate for LIBs, and the bioinspired design in structure will play an increasingly important role in the development of high-performance battery in the future. [ABSTRACT FROM AUTHOR]