Lightweight, ultrathin, and flexible electromagnetic interference (EMI) shielding materials with high electromagnetic shielding effectiveness (SE) and excellent mechanical robustness are greatly desired for miniaturized and highly integrated electronics. Herein, for the first time, a freestanding, ultrathin, and flexible Ti3C2T x /poly­(3,4-ethylenedioxythiophene)–poly­(styrenesulfonate) (PEDOT:PSS) composite film with a “brick-and-mortar” structure is biomimetically designed and fabricated via a vacuum-assisted filtration process. The ultrathin polymeric composite film with a weight ratio 7:1 of Ti3C2T x to PEDOT:PSS is only 11.1 μm in thickness but exhibits a high EMI SE value of 42.10 dB. Meanwhile, the tensile strength increases considerably from 5.62 to 13.71 MPa and the corresponding ruptured strain increases from 0.18 to 0.29% compared with pure Ti3C2T x MXene film, respectively. Moreover, the hybrid film displays a superior conductivity of 340.5 S/cm and an outstanding specific EMI shielding efficiency of 19 497.8 dB cm2 g–1. The superior electrical conductivity and specific EMI shielding efficiency imply the excellent potential of the Ti3C2T x /PEDOT:PSS composite films for ultrathin, lightweight, and flexible EMI shielding materials.

A free-standing lithium titanate (Li4Ti5O12)/carbon nanotube/cellulose nanofiber hybrid network film is successfully assembled by using a pressure-controlled aqueous extrusion process, which is highly efficient and easily to scale up from the perspective of disposable and recyclable device production. This hybrid network film used as a lithium-ion battery (LIB) electrode has a dual-layer structure consisting of Li4Ti5O12/carbon nanotube/cellulose nanofiber composites (hereinafter referred to as LTO/CNT/CNF), and carbon nanotube/cellulose nanofiber composites (hereinafter referred to as CNT/CNF). In the heterogeneous fibrous network of the hybrid film, CNF serves simultaneously as building skeleton and a biosourced binder, which substitutes traditional toxic solvents and synthetic polymer binders. Of importance here is that the CNT/CNF layer is used as a lightweight current collector to replace traditional heavy metal foils, which therefore reduces the total mass of the electrode while keeping the same areal loading of active materials. The free-standing network film with high flexibility is easy to handle, and has extremely good conductivity, up to 15.0 S cm(-1). The flexible paper-electrode for LIBs shows very good high rate cycling performance, and the specific charge/discharge capacity values are up to 142 mAh g(-1) even at a current rate of 10 C. On the basis of the mild condition and fast assembly process, a CNF template fulfills multiple functions in the fabrication of paper-electrode for LIBs, which would offer an ever increasing potential for high energy density, low cost, and environmentally friendly flexible electronics.

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Highly efficient EMI shielding composite films with excellent flexibility were fabricated by intercalating sliver nanowires into Ti3C2Tx nanosheets using nanocellulose as a green binder.

Flexible free-standing carbonized cellulose-based hybrid film is integrately designed and served both as paper anode and as lightweight current collector for lithium-ion batteries. The well-supported heterogeneous nanoarchitecture is constructed from Li4Ti5O12 (LTO), carbonized cellulose nanofiber (C-CNF) and carbon nanotubes (CNTs) using by a pressured extrusion papermaking method followed by in situ carbonization under argon atmospheres. The in situ carbonization of CNF/CNT hybrid film immobilized with uniform-dispersed LTO results in a dramatic improvement in the electrical conductivity and specific surface area, so that the carbonized paper anode exhibits extraordinary rate and cycling performance compared to the paper anode without carbonization. The flexible, lightweight, single-layer cellulose-based hybrid films after carbonization can be utilized as promising electrode materials for high-performance, low-cost, and environmentally friendly lithium-ion batteries.

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