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The sluggish anodic oxygen evolution reaction (OER) in proton exchange membrane (PEM) electrolysis necessitates applied bias to facilitate electron transfer as well as bond cleavage and formation. Traditional electrocatalysis focuses on analyzing the effects of electron transfer, while the role of charge accumulation induced by the applied overpotential has not been thoroughly investigated. To explore the influence mechanism of bias-driven charge accumulation, capacitive Mn is incorporated into IrO 2 to regulate the local electronic structure and the adsorption behavior. The applied bias triggers dynamic redox reactions at the active sites, which introduce local charge accumulation on the surface of electrocatalyst. Under bias, Mn oxidation induced a noticeable pseudocapacitance in the pre-OER region, promoting the OER kinetics of iridium sites. Meanwhile, the increased oxygen vacancy formation energy further prevents the lattice oxygen activation. The PEM electrolyzer, equipped with optimal materials as an anode, operates at a low driving voltage of 1.637 V under 2.0 A cm -2 , maintaining stable performance for over 800 h with a low degradation rate (19.4 µV h -1 ). This work provides insights into the performance of metal oxide catalysts in acidic environments and offers forward-looking strategies for enhancing the catalytic performance through dynamic redox induced capacitive behavior., (© 2024 Wiley‐VCH GmbH.)

Iridium (Ir)-based oxide is the state-of-the-art electrocatalyst for acidic water oxidation, yet it is restricted to a few Ir-O octahedral packing modes with limited structural flexibility. Herein, the geometric structure diversification of Ir is achieved by integrating spatially correlated Ir atoms into the surface lattice of TiO 2 and its booting effect on oxygen evolution reaction (OER) is investigated. Notably, the resultant i-Ir/TiO 2 catalyst exhibits much higher electrocatalytic activity, with an overpotential of 240 mV at 10 mA cm -2 and excellent stability of 315 h at 100 mA cm -2 in acidic electrolyte. Both experimental and theoretical findings reveal that flexible Ir─O─Ir coordination with varied geometric structure plays a crucial role in enhancing OER activity, which optimize the intermediate adsorption by adjusting the d-band center of active Ir sites. Operando characterizations demonstrate that the interactive Ir─O─Ir units can suppress over-oxidation of Ir, effectively widening the stable region of Ir species during the catalytic process. The proton exchange membrane (PEM) electrolyzer, equipped with i-Ir/TiO 2 as an anode, gives a low driving voltage of 1.63 V at 2 A cm -2 and maintains stable performance for over 440 h. This work presents a general strategy to eliminate the inherent geometric limitations of IrO x species, thereby inspiring further development of advanced catalyst designs., (© 2024 Wiley‐VCH GmbH.)

β-CaSiO 3 based glass-ceramics are among the most reliable materials for electronic packaging. However, developing a CaSiO 3 glass-ceramic substrate with both high strength (>230 MPa) and low dielectric constant (<5) remains challenging due to its polycrystalline nature. The present work has succeeded in synthesizing single-crystalline β-CaSiO 3 for a high-performance glass-ceramic substrate. This is accomplished by introducing Al 3+ into the CaO-B 2 O 3 -SiO 2 glass system, and by optimizing the sintering condition. Al 3+ doping facilitates a heterogeneous network structure that energetically favors the precipitation of polycrystalline particles, including nanosized β-CaSiO 3 crystals and sub-nanosized α-CaSiO 3 crystals. As the sintering temperature increases, the nano α-CaSiO 3 crystals (2-10 nm) are gradually absorbed by the β-CaSiO 3 crystals. Through atomic rearrangement, α-CaSiO 3 crystals transform into micrometer-sized single crystal β-CaSiO 3 (1-2 µm) with layered structure. The low temperature co-fired β-CaSiO 3 glass-ceramics exhibit exceptional properties, including a low dielectric constant of 4.04, a low dielectric loss of 3.15 × 10 -3 at 15 GHz, and a high flexural strength of 256 MPa. This work provides a new strategy for fabricating high-performance single-crystalline glass-ceramics for electronic packaging and other applications., (© 2024 Wiley‐VCH GmbH.)

The recovery of precious metals (PMs) from secondary resources has garnered significant attention due to environmental and economic considerations. Covalent organic frameworks (COFs) have emerged as promising adsorbents for this purpose, owing to their tunable pore size, facile functionalization, exceptional chemical stability, and large specific surface area. This review provides an overview of the latest research progress in utilizing COFs to recover PMs. Firstly, the design and synthesis strategies of chemically stable COF-based materials, including pristine COFs, functionalized COFs, and COF-based composites, are delineated. Furthermore, the application of COFs in the recovery of gold, silver, and platinum group elements is delved into, emphasizing their high adsorption capacity and selectivity as well as recycling ability. Additionally, various interaction mechanisms between COFs and PM ions are analyzed. Finally, the current challenges faced by COFs in the field of PM recovery are discussed, and potential directions for future development are proposed, including enhancing the recyclability and reusability of COF materials and realizing the high recovery of PMs from actual acidic wastewater. With the targeted development of COF-based materials, the recovery of PMs can be realized more economically and efficiently in the future., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Water oxidation, or the oxygen evolution reaction (OER), which combines two oxygen atoms from two water molecules and releases one oxygen molecule, plays the key role by providing protons and electrons needed for the hydrogen generation, electrochemical carbon dioxide reduction, and nitrogen fixation. The multielectron transfer OER process involves multiple reaction intermediates, and a high overpotential is needed to overcome the sluggish kinetics. Among the different water splitting devices, proton exchange membrane (PEM) water electrolyzer offers greater advantages. However, current anode OER electrocatalysts in PEM electrolyzers are limited to precious iridium and ruthenium oxides. Developing highly active, stable, and precious-metal-free electrocatalysts for water oxidation in acidic media is attractive for the large-scale application of PEM electrolyzers. In recent years, various types of precious-metal-free catalysts such as carbon-based materials, earth-abundant transition metal oxides, and multiple metal oxide mixtures have been investigated and some of them show promising activity and stability for acidic OER. In this review, the thermodynamics of water oxidation, Pourbaix diagram of metal elements in aqueous solution, and theoretical screening and prediction of precious-metal-free electrocatalysts for acidic OER are first elaborated. The catalytic performance, reaction kinetics, and mechanisms together with future research directions regarding acidic OER are summarized and discussed., (© 2021 Wiley-VCH GmbH.)

Certain chemotherapeutics and forms of ionizing radiation can induce immunogenic cell death (ICD). If there simultaneously exist immune adjuvants within the tumor, such antitumor immunity would be further amplified. However, as clinical chemo/radiotherapies are usually repeatedly given at low individual doses, it would be impractical to administrate immune adjuvants into tumors at each dose of chemo/radiotherapies. Thus, a smart hydrogel is developed that releases immune adjuvants in response to repeatedly applied chemo-/radiotherapies. Herein, alginate is conjugated with an adenosine triphosphate (ATP)-specific aptamer, which is hybridized with immunoadjuvant CpG oligonucleotide. Upon intratumoral injection, alginate-based hydrogel is formed in situ. Interestingly, low doses of oxaliplatin or X-rays, while inducing ICD of tumor cells, could trigger release of ATP, which competitively binds with ATP-specific aptamer to trigger CpG release. Therefore, the smart hydrogel could release the immune adjuvant synchronized with low-dose repeated chemo/radiotherapies, achieving remarkable synergistic responses in eliminating established tumors, as well as immune memory to reject re-challenged tumors. Moreover, repeated radiotherapies assisted by the smart hydrogel could inhibit distant tumor metastases, especially in combination with immune checkpoint blockade. The study presents a conceptually new strategy to boost cancer immunotherapy coherent with repeated low-dose chemo-/radiotherapies following a clinically relevant manner., (© 2021 Wiley-VCH GmbH.)

Inflammation is a common cause of many acute and chronic inflammatory diseases. A major limitation of existing anti-inflammatory therapeutics is that they cannot simultaneously regulate pro-inflammatory cytokine production, oxidative stress, and recruitment of neutrophils and macrophages. To overcome this limitation, nanoparticles (NPs) with multiple pharmacological activities are synthesized, using a chemically modified cyclic oligosaccharide. The manufacture of this type of bioactive, saccharide material-based NPs (defined as LCD NP) is straightforward, cost-effective, and scalable. Functionally, LCD NP effectively inhibits inflammatory response, oxidative stress, and cell migration for both neutrophils and macrophages, two major players of inflammation. Therapeutically, LCD NP shows desirable efficacies for the treatment of acute and chronic inflammatory diseases in mouse models of peritonitis, acute lung injury, and atherosclerosis. Mechanistically, the therapeutic benefits of LCD NP are achieved by inhibiting neutrophil-mediated inflammatory macrophage recruitment and by preventing subsequent pro-inflammatory events. In addition, LCD NP shows good safety profile in a mouse model. Thus, LCD NP can serve as an effective anti-inflammatory nanotherapy for the treatment of inflammatory diseases mainly associated with neutrophil and macrophage infiltration., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

NiFe-based layered double hydroxides (LDHs) are among the most efficient oxygen evolution reaction (OER) catalysts in alkaline medium, but their long-term OER stabilities are questionable. In this work, it is demonstrated that the layered structure makes bulk NiFe LDH intrinsically not stable in OER and the deactivation mechanism of NiFe LDH in OER is further revealed. Both operando electrochemical and structural characterizations show that the interlayer basal plane in bulk NiFe LDH contributes to the OER activity, and the slow diffusion of proton acceptors (e.g., OH - ) within the NiFe LDH interlayers during OER causes dissolution of NiFe LDH and therefore decrease in OER activity with time. To improve diffusion of proton acceptors, it is proposed to delaminate NiFe LDH into atomically thin nanosheets, which is able to effectively improve OER stability of NiFe LDH especially at industrial operating conditions such as elevated operating temperatures (e.g., at 80 °C) and large current densities (e.g., at 500 mA cm -2 )., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The implementation of water splitting systems, powered by sustainable energy resources, appears to be an attractive strategy for producing high-purity H 2 in the absence of the release of carbon dioxide (CO 2 ). However, the high cost, impractical operating conditions, and unsatisfactory efficiency and stability of conventional methods restrain their large-scale development. Seawater covers 70% of the Earth's surface and is one of the most abundant natural resources on the planet. New research is looking into the possibility of using seawater to produce hydrogen through electrolysis and will provide remarkable insight into sustainable H 2 production, if successful. Here, guided by density functional theory (DFT) calculations to predict the selectivity of gas-evolving catalysts, a seawater-splitting device equipped with affordable state-of-the-art electrocatalysts composed of earth-abundant elements (Fe, Co, Ni, and Mo) is demonstrated. This device shows excellent durability and specific selectivity toward the oxygen evolution reaction in seawater with near 100% Faradaic efficiency for the production of H 2 and O 2 . Powered by a single commercial III-V triple-junction photovoltaic cell, the integrated system achieves spontaneous and efficient generation of high-purity H 2 and O 2 from seawater at neutral pH with a remarkable 17.9% solar-to-hydrogen efficiency., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

While glasses formed by quenching the molten states of inorganic non-metallic, organic, and metallic species are known, those containing both inorganic and organic moieties are far less prevalent. Network materials consisting of inorganic nodes linked by organic ligands do however exist in the crystalline or amorphous domain. This large family of open framework compounds, called metal-organic frameworks (MOFs) or coordination polymers, has been investigated intensively in the past two decades for a variety of applications, almost all of which stem from their high internal surface areas and chemical versatility. Recently, a selection of MOFs has been demonstrated to undergo melting and vitrification upon cooling. Here, these recent discoveries and the connections between the fields of MOF chemistry and glass science are summarized. Possible advantages and applications for MOF glasses produced by utilizing the tunable chemistry of the crystalline state are also highlighted., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The combination of water-based titanate nanosheets dispersion and silk fibroin solution allows the realization of a versatile nanocomposite. Different fabrication techniques can be easily applied on these nanocomposites to manipulate the end form of these materials on the micro- and nanoscale. Easy tunability of the refractive index from n = 1.55 up to n = 1.97 is achieved, making it attractive for flexible, biopolymer-based optical devices., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A formulation of regenerated silk fibroin solution that can be easily functionalized and inkjet printed on numerous surfaces is developed. As an example, the inks can be printed on laboratory gloves that change color when exposed to bacteria., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Pt-Ni alloy nanoparticles are synthesized and used as counter electrodes in dye-sensitized solar cells (DSSCs) for the first time. A PCE of 9.15% is achieved with the Pt3 Ni counter electrode, displaying an evident improvement compared with the conventional pure Pt (8.33%). The cell stability is also obviously increased with the Pt3 Ni counter electrode., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Materials, device designs and manufacturing approaches are presented for classes of RF electronic components that are capable of complete dissolution in water or biofluids. All individual passive/active components as well as system-level examples such as wireless RF energy harvesting circuits exploit active materials that are biocompatible. The results provide diverse building blocks for physically transient forms of electronics, of particular potential value in bioresorbable medical implants with wireless power transmission and communication capabilities., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Protein-protein imprinting of silk fibroin is introduced as a rapid, high-throughput method for the fabrication of nanoscale structures in silk films, through the application of heat and pressure. Imprinting on conformal surfaces is demonstrated with minor adjustments to the system, at resolutions comparable to other currently available nonplanar nanoimprint lithography techniques., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

By a reusable transfer fabrication technique, we demonstrate high-fidelity fabrication of metal nanoparticles, optical nanoantennas, and nanohole arrays directly on a functional silk biopolymer. The ability to reproducibly pattern silk biopolymers with arbitrarily complex plasmonic arrays is of importance for a variety of applications in optical biosensing, tissue engineering, cell biology, and the development of novel bio-optoelectronic medical devices., (Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

This review addresses the use of silk protein as a sustainable material in optics and photonics, electronics and optoelectronic applications. These options represent additional developments for this technology platform that compound the broad utility and impact of this material for medical needs that have been recently described in the literature. The favorable properties of the material certainly make a favorable case for the use of silk, yet serve as a broad inspiration to further develop biological foundries for both the synthesis and processing of Nature's materials for technological applications., (Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

An array of passive metamaterial antennas fabricated on all protein-based silk substrates were conformally transferred and adhered to the surface of an apple. This process allows the opportunity for intimate contact of micro- and nanostructures that can probe, and accordingly monitor changes in, their surrounding environment. This provides in situ monitoring of food quality. It is to be noted that this type of sensor consists of all edible and biodegradable components, holding utility and potential relevance for healthcare and food/consumer products and markets., (Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Supercapacitor electrode materials: Carbon nanocages are conveniently produced by an in situ MgO template method and demonstrate high specific capacitance over a wide range of charging-discharging rates with high stability, superior to the most carbonaceous supercapacitor electrode materials to date. The large specific surface area, good mesoporosity, and regular structure are responsible for the excellent performance., (Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Pt-Co alloyed nanoparticles can be facilely immobilized onto CNx nanotubes due to the incorporated nitrogen, report Yanwen Ma, Zheng Hu, and co-workers on p. 4953. The as-prepared electrocatalysts exhibit good performance for oxygen reduction reactions in acidic media arising from the high dispersion and alloying effect of Pt-Co nanoparticles, as well as the intrinsic catalytic capacity of CNx nanotubes, which is significant for the development of fuel cells., (Copyright © 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A straight forward method for immobilizing Pt-Co alloyed nanoparticles onto nitrogen-doped CNx nanotubes is presented. The as-prepared electrocatalysts exhibit good performance for oxygen reduction reaction in acidic medium arising from the high-dispersion and alloying effect of the Pt-Co nanoparticles and the intrinsic catalytic capacity of the CNx nanotubes., (Copyright © 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)