Advanced Materials

Xu, Rong; Bhangu, Sukhvir Kaur; Sourris, Karly C.; Vanni, Domitilla; Sani, Marc‐Antoine; Karas, John A.; Alt, Karen; Niego, Be'eri; Ale, Anukreity; Besford, Quinn A.; Dyett, Brendan; Patrick, Joshua; Carmichael, Irena; Shaw, Jonathan E.; Caruso, Frank; Cooper, Mark E.; Hagemeyer, Christoph E.; Cavalieri, Francesca

doi: 10.1002/adma.202210392pmid: 36908046

Glucose‐responsive insulin‐delivery platforms that are sensitive to dynamic glucose concentration fluctuations and provide both rapid and prolonged insulin release have great potential to control hyperglycemia and avoid hypoglycemia diabetes. Here, biodegradable and charge‐switchable phytoglycogen nanoparticles capable of glucose‐stimulated insulin release are engineered. The nanoparticles are “nanosugars” bearing glucose‐sensitive phenylboronic acid groups and amine moieties that allow effective complexation with insulin (≈95% loading capacity) to form nanocomplexes. A single subcutaneous injection of nanocomplexes shows a rapid and efficient response to a glucose challenge in two distinct diabetic mouse models, resulting in optimal blood glucose levels (below 200 mg dL–1) for up to 13 h. The morphology of the nanocomplexes is found to be key to controlling rapid and extended glucose‐regulated insulin delivery in vivo. These studies reveal that the injected nanocomplexes enabled efficient insulin release in the mouse, with optimal bioavailability, pharmacokinetics, and safety profiles. These results highlight a promising strategy for the development of a glucose‐responsive insulin delivery system based on a natural and biodegradable nanosugar.

Chu, Youqi; Mu, Yongbiao; Zou, Lingfeng; Hu, Yan; Cheng, Jie; Wu, Buke; Han, Meisheng; Xi, Shibo; Zhang, Qing; Zeng, Lin

doi: 10.1002/adma.202212308pmid: 36913606

Pushing the limit of cutoff potentials allows nickel‐rich layered oxides to provide greater energy density and specific capacity whereas reducing thermodynamic and kinetic stability. Herein, a one‐step dual‐modified method is proposed for in situ synthesizing thermodynamically stable LiF&FeF3 coating on LiNi0.8Co0.1Mn0.1O2 surfaces by capturing lithium impurity on the surface to overcome the challenges suffered. The thermodynamically stabilized LiF&FeF3 coating can effectively suppress the nanoscale structural degradation and the intergranular cracks. Meanwhile, the LiF&FeF3 coating alleviates the outward migration of Oα− (α<2), increases oxygen vacancy formation energies, and accelerates interfacial Li+ diffusion. Benefited from these, the electrochemical performance of LiF&FeF3 modified materials is improved (83.1% capacity retention after 1000 cycles at 1C), even under exertive operational conditions of elevated temperature (91.3% capacity retention after 150 cycles at 1C). This work demonstrates that the dual‐modified strategy can simultaneously address the problems of interfacial instability and bulk structural degradation and represents significant progress in developing high‐performance lithium‐ion batteries (LIBs).

Xie, Zongliang; Zhang, Xiayu; Xiao, Yuxin; Wang, Hailan; Shen, Mingyao; Zhang, Simin; Sun, Haodong; Huang, Rongjuan; Yu, Tao; Huang, Wei

doi: 10.1002/adma.202212273pmid: 36896893

Organic mechanoluminescent (ML) materials possessing photophysical properties that are sensitive to multiple external stimuli have shown great potential in many fields, including optic and sensing. Particularly, the photoswitchable ML property for these materials is fundamental to their applications but remains a formidable challenge. Herein, photoswitchable ML is successfully realized by endowing reversible photochromic properties to an ML molecule, namely 2‐(1,2,2‐triphenylvinyl) fluoropyridine (o‐TPF). o‐TPF shows both high‐contrast photochromism with a distinct color change from white to purplish red, as well as bright blue ML (λML = 453 nm). The ML property can be repeatedly switched between ON and OFF states under alternate UV and visible light irradiation. Impressively, the photoswitchable ML is of high stability and repeatability. The ML can be reversibly switched on and off by conducting alternate UV and visible light irradiation in cycles under ambient conditions. Experimental results and theoretical calculations reveal that the change of dipole moment of o‐TPF during the photochromic process is responsible for the photoswitchable ML. These results outline a fundamental strategy to achieve for the control of organic ML and pave the way to the development of expanded smart luminescent materials and their applications.

Wang, Xin‐Yi; Yu, Zi‐Di; Lu, Yang; Yao, Ze‐Fan; Zhou, Yang‐Yang; Pan, Chen‐Kai; Liu, Yi; Wang, Zi‐Yuan; Ding, Yi‐Fan; Wang, Jie‐Yu; Pei, Jian

doi: 10.1002/adma.202300634pmid: 36905682

Ma, Jiangping; Xiong, Xin; Wu, Di; Wang, Yang; Ban, Chaogang; Feng, Yajie; Meng, Jiazhi; Gao, Xingsen; Dai, Ji‐Yan; Han, Guang; Gan, Li‐Yong; Zhou, Xiaoyuan

doi: 10.1002/adma.202300027pmid:

Yu, Le; Huang, Jing; Wang, Sijun; Qi, Luhe; Wang, Shanshan; Chen, Chaoji

doi: 10.1002/adma.202210789pmid: 36848503

The strong reactivity of water in aqueous electrolytes toward metallic zinc (Zn), especially at aggressive operating conditions, remains the fundamental obstacle to the commercialization of aqueous zinc metal batteries (AZMBs). Here, a water‐immiscible ionic liquid diluent 1‐ethyl‐3‐methylimidazolium bis(fluorosulfonyl)amide (EmimFSI) is reported that can substantially suppress the water activity of aqueous electrolyte by serving as a “water pocket”, enveloping the highly active H2O‐dominated Zn2+ solvates and protecting them from parasitic reactions. During Zn deposition, the cation Emim+ and anion FSI− function respectively in mitigating the tip effect and regulating the solid electrolyte interphase (SEI), thereby favoring a smooth Zn deposition layer protected by inorganic species‐enriched SEI featuring high uniformity and stability. Combined with the boosted chemical/electrochemical stability endowed by the intrinsic merits of ionic liquid, this ionic liquid‐incorporated aqueous electrolyte (IL‐AE) enables the stable operation of Zn||Zn0.25V2O5·nH2O cells even at a challenging temperature of 60 °C (>85% capacity retention over 400 cycles). Finally, as an incidental but practically valuable benefit, the near‐zero vapor pressure nature of ionic liquid allows the efficient separation and recovery of high‐value components from the spent electrolyte via a mild and green approach, promising the sustainable future of IL‐AE in realizing practical AZMBs.

Nazari, Pariya; Bäuerle, Rainer; Zimmermann, Johannes; Melzer, Christian; Schwab, Christopher; Smith, Anna; Kowalsky, Wolfgang; Aghassi‐Hagmann, Jasmin; Hernandez‐Sosa, Gerardo; Lemmer, Uli

doi: 10.1002/adma.202212189pmid: 36872845

Highly sensitive microfiber strain sensors are promising for the detection of mechanical deformations in applications where limited space is available. In particular for in situ battery thickness monitoring where high resolution and low detection limit are key requirements. Herein, the realization of a highly sensitive strain sensor for in situ lithium‐ion (Li‐ion) battery thickness monitoring is presented. The compliant fiber‐shaped sensor is fabricated by an upscalable wet‐spinning method employing a composite of microspherical core‐shell conductive particles embedded in an elastomer. The electrical resistance of the sensor changes under applied strain, exhibiting a high strain sensitivity and extremely low strain detection limit of 0.00005 with high durability of 10 000 cycles. To demonstrate the accuracy and ease of applicability of this sensor, the real‐time thickness change of a Li‐ion battery pouch cell is monitored during the charge and discharge cycles. This work introduces a promising approach with the least material complexity for soft microfiber strain gauges.

Qiao, Haiyan; Sun, Shengtong; Wu, Peiyi

doi: 10.1002/adma.202300593pmid: 36861380

Humans use periodically ridged fingertips to precisely perceive the characteristics of objects via ion‐based fast‐ and slow‐adaptive mechanotransduction. However, designing artificial ionic skins with fingertip‐like tactile capabilities remains challenging because of the contradiction between structural compliance and pressure sensing accuracy (e.g., anti‐interference from stretch and texture recognition). Inspired by the formation and modulus‐contrast hierarchical structure of fingertips, an aesthetic ionic skin grown from a non‐equilibrium Liesegang patterning process is introduced. This ionic skin with periodic stiff ridges embedded in a soft hydrogel matrix enables strain‐undisturbed triboelectric dynamic pressure sensing as well as vibrotactile texture recognition. By coupling with another piezoresistive ionogel, an artificial tactile sensory system is further fabricated as a soft robotic skin to mimic the simultaneous fast‐ and slow‐adaptive multimodal sensations of fingers in grasping actions. This approach may inspire the future design of high‐performance ionic tactile sensors for intelligent applications in soft robotics and prosthetics.

Hood, Zachary D.; Mane, Anil U.; Sundar, Aditya; Tepavcevic, Sanja; Zapol, Peter; Eze, Udochukwu D.; Adhikari, Shiba P.; Lee, Eungje; Sterbinsky, George E.; Elam, Jeffrey W.; Connell, Justin G.

doi: 10.1002/adma.202300673pmid: 36929566

Sulfide‐based solid‐state electrolytes (SSEs) exhibit many tantalizing properties including high ionic conductivity and favorable mechanical properties for next‐generation solid‐state batteries. Widespread adoption of these materials is hindered by their intrinsic instability under ambient conditions, which makes them difficult to process at scale, and instability at the Li||SSE and cathode||SSE interfaces, which limits cell performance and lifetime. Atomic layer deposition is leveraged to grow thin Al2O3 coatings on Li6PS5Cl powders to address both issues simultaneously. These coatings can be directly grown onto Li6PS5Cl particles with negligible chemical modification of the underlying material and enable exposure of powders to pure and H2O‐saturated oxygen environments for ≥4 h with minimal reactivity, compared with significant degradation of the uncoated powder. Pellets fabricated from coated powders exhibit ionic conductivities up to 2× higher than those made from uncoated material, with a simultaneous decrease in electronic conductivity and significant suppression of chemical reactivity at the Li‐SSE interface. These benefits result in significantly improved room temperature cycle life at high capacity and current density. It is hypothesized that this enhanced performance derives from improved intergranular properties and improved Li metal adhesion. This work points to a completely new framework for designing active, stable, and scalable materials for next‐generation solid‐state batteries.

Li, Zheng; Zou, Jianhua; Chen, Xiaoyuan

doi: 10.1002/adma.202209529pmid: 36445169

Emerging as a potent anticancer treatment, subcellular targeted cancer therapy has drawn increasing attention, bringing great opportunities for clinical application. Here, two targeting strategies for four main subcellular organelles (mitochondria, lysosome, endoplasmic reticulum, and nucleus), including molecule‐ and nanomaterial (inorganic nanoparticles, micelles, organic polymers, and others)‐based targeted delivery or therapeutic strategies, are summarized. Phototherapy, chemotherapy, radiotherapy, immunotherapy, and “all‐in‐one” combination therapy are among the strategies covered in detail. Such materials are constructed based on the specific properties and relevant mechanisms of organelles, enabling the elimination of tumors by inducing dysfunction in the corresponding organelles or destroying specific structures. The challenges faced by organelle‐targeting cancer therapies are also summarized. Looking forward, a paradigm for organelle‐targeting therapy with enhanced therapeutic efficacy compared to current clinical approaches is envisioned.