3D Printed Li–S Batteries with In Situ Decorated Li₂S/C Cathode: Interface Engineering Induced Loading‐Insensitivity for Scaled Areal Performance

Abstract

Holding manifold advantages including environmental benignity, enhanced structural robustness, and high capacity, Li2S as a competitive substitute of sulfur in Li–S batteries is receiving escalating attention. However, serious issues rooted in its intrinsic poor conductivity and sluggish mass transport present the significant challenge of achieving high active material use with appealing kinetics for effective scaling in areal capacitance under elevated loading densities. This renders current Li2S cathodes incapable of securing energy availability that responds to power‐hungry modern electronics. Here for the first time, an interfacial engineering approach is devised by in situ decorating a 3D printed carbonaceous scaffold with uniform surface‐deposited Li2S and by healing the printed adjacent interface to eliminate the interfacial resistance. As a result, facile mass transport throughout the whole printed matrix is enabled. 3D printed electrodes with high active material use and loading‐insensitive performance delivering outstanding areal capacity and fast kinetics of 6.29 mAh cm−2 at 6 mA cm−2 under an impressive loading density of 10 mg cm−2 are realized, which are among the best results reported for Li2S‐based batteries. The thrilling performance points to a highly effective approach that advances the performance of Li2S cathodes closer toward real‐world applications.

3D Printing Architecting Reservoir‐Integrated Anode for Dendrite‐Free, Safe, and Durable Zn Batteries

“…Meanwhile, as shown in Figure S1b (Supporting Information), the plateau separation of the storage modulus (G') that masters the original solid shape and the loss modulus (G'') that reflects the irreversible energy loss is distinct, and the much higher G' over G'' before the yield point manifests a solid behavior to maintain the required shape after completing consistent printing under shear stress beyond the yield point. [29,30] After 3D printing, a two-layer reservoirintegrated structure with a 400 µm interval in-betweens is readily established. The following heat-treatment decomposes the nitrogen precursor, and the final N-doped 3D printed carbon host is named as 3DP-NC.…”

Ion‐Inserted Metal–Organic Frameworks Accelerate the Mass Transfer Kinetics in Lithium–Sulfur Batteries

“…The first intersection of the Nyquist plots with real axis at high frequency and the semicircle at the medium frequency correspond to the electronic resistance ( R e ) equivalent component and charge transfer resistance ( R ct ), respectively (Figure 4g). [ 38 ] The R e of the battery with Li‐MOF/RGO (4.4 Ω) is slightly lower than those of the battery with MOF/RGO (5.0 Ω) and with RGO (5.1 Ω). Significantly, the R ct of the battery with Li‐MOF/RGO (6.8 Ω) is also much lower than those of battery with MOF/RGO (9.0 Ω) and RGO (14.2 Ω), indicating facilitated conversion kinetics by introducing Li + inserted MOF.…”

Current advances and future perspectives of additive manufacturing for functional polymeric materials and devices

“…The encouraged mass transport by the structure as well as interface design, in turn, led to loading-insensitivity and linearly scaled areal capacity up to an impressive value of 6.29 mAh/cm 2 at a large current density of 6 mA/cm 2 . 98 Apart from batteries, supercapacitors with advanced performance have also been reported by utilizing DIW. A similar strategy used concentrated GO as a rheological modifier while incorporated CNT and activated carbon (AC) inside the conductive matrix to enhance conductivity, and electrosorption sites were reported ( Figure 5F).…”

“…A 3D open lattice conductive scaffold was printed and in‐situ decorated by uniformly dispersed Li 2 S tightly interfacing with the underlying conductor. The encouraged mass transport by the structure as well as interface design, in turn, led to loading‐insensitivity and linearly scaled areal capacity up to an impressive value of 6.29 mAh/cm 2 at a large current density of 6 mA/cm 2 98 …”