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Advances in adaptive immunity have greatly contributed to the development of cancer immunotherapy. However, its over-low efficacy and insufficient invasion of immune cells in the tumor tissue, and safety problems caused by cytokine storm, have seriously impeded further clinical application for solid tumor immunotherapy. Notably, the immune microenvironment of the lungs is naturally enriched with alveolar macrophages (AMs). Herein, we introduce a novel nebulized magnetothermal immunotherapy strategy to treat orthotopic lung cancer by using magnetothermal nanomaterial (Zn-CoFe2O4@Zn-MnFe2O4-PEG, named ZCMP), which can release iron ions via an acid/thermal-catalytic reaction to maximize the use of lung's immune environment through the cascade activations of AMs and natural killer (NK) cells. Nebulized administration greatly enhance drug bioavailability by localized drug accumulation at the lesion site. Upon mild magnetic hyperthermia, the released iron ions catalyze endogenous H2O2 decomposition to produce reactive oxygen species (ROS), which triggers the M1 polarization of AMs, and the resultant inflammatory cytokine IFN-β, IL-1β and IL-15 releases to activate c-Jun, STAT5 and GZMB related signaling pathways, promoting NK cells proliferation and activation. This innovative strategy optimally utilizes the lung's immune environment and shows excellent immunotherapeutic outcomes against orthotopic lung cancer., (© 2024 Wiley‐VCH GmbH.)

Electrochemical nitrate reduction reaction (NO3-RR) has promising prospects for green synthesis of ammonia and environmental remediation. However, the performance of catalysts at high current density usually suffers from the high energy barrier for the nitrate (NO3-) to nitrite (NO2-) and the competitive hydrogen evolution. Herein, we proposed a two-step relay mechanism through spontaneous redox reaction followed electrochemical reaction by introducing low-valence Fe species into Ni2P nanosheets to significantly enhance the NO3-RR performance at industrial current density. The existence of low-valence Fe species bypasses the NO3- to NO2- step through the spontaneous redox with NO3- to produce NO2- and Fe2O3, regulates the electronic structure of Ni2P to reduce the barrier of NO2- to NH3, thirdly prohibits the hydrogen evolution by consuming the excess active hydrogen through reduction of Fe2O3 to recover low-valence Fe species. The triple regulations via Fe redox during the two-step relay reactions guarantee the Fe-Ni2P@NF high ammonia yield of 120.1 mg h-1 cm-2 with Faraday efficiency of more than 90% over a wide potential window and a long-term stability of more than 130 h at ~1000 mA cm-2. This work provides a new strategy to realize the design and synthesis of nitrate reduction electrocatalysts at high current densities., (© 2024 Wiley‐VCH GmbH.)

The photocatalytic cycloaddition reaction between CO2 and epoxide is one of the most promising green routes for CO2 utilization, for which high performance photocatalysts are intensely desired. Herein, we have constructed an S-scheme heterojunction of MIL-125@ZIF-67 modified by amino groups, which achieves a cyclic carbonate yield of as high as 99% without employing any co-catalyst, outperforming the previously reported photocatalysts. In-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and in-situ electron paramagnetic resonance (EPR) spectroscopy reveal the important role of photogenerated electron migration from Lewis acid (Co) sites to the O atom of epoxide in triggering its ring-opening (the rate-determining step of CO2 cycloaddition reaction) under the assistance of photogenerated hole. Synergistically and concurrently, the Lewis base (amino groups) sites activate CO2 to CO2*, facilitating the following CO2 cycloaddition. Such a synergistic effect provides a most favorable approach to design efficient heterogeneous photocatalysts with dual/multiple-active sites for CO2 cycloaddition reaction., (© 2024 Wiley‐VCH GmbH.)

Plastic pollution, an increasingly serious global problem, can be addressed through the full lifecycle management of plastics, including plastics recycling as one of the most promising approaches. System design, catalyst development, and product separation are the keys in improving the economics of electrocatalytic plastics recycling. Here, a membrane-free co-production system was devised to produce succinic acid (SA) at both anode and cathode respectively by the co-electrolysis of polybutylene succinate (PBS) waste plastics and biomass-derived maleic acid (MA) for the first time. To this end, Cr3+-Ni(OH)2 electrocatalyst featuring much enhanced 1,4-butanediol (BDO) oxidation reaction (BOR) activity has been synthesized and the role of doped Cr has been revealed as an "electron puller" to accelerate the rate-determining step (RDS) in the Ni2+/Ni3+ cycling. Impressively, an extra-high SA production rate of 3.02 g h-1 and ultra-high apparent Faraday efficiency towards SA (FEapparent=181.5%) have been obtained. A carbon dioxide-assisted sequential precipitation approach has been developed to produce high-purity SA and byproduct NaHCO3 solids. Preliminary techno-economic analysis demonstrates that the reported system is economically profitable and promising for future industrial applications., (© 2024 Wiley‐VCH GmbH.)

Soft ionic elastomers that are self-healable, fatigue-free, and environment-tolerant are ideal structural and sensing materials for artificial prosthetics, soft electronics, and robotics to survive unpredictable service conditions. However, most synthetic strategies failed to unite rapid healing, fatigue resistance, and environmental robustness, limited by their singular compositional/structural designs. Here, we present a soft, tough, fatigue-resistant, and self-healable ionic elastomer (STFSI elastomer), which fuses skin-like binary assembly and Bouligand helicoidal structure into a composite of thermoplastic polyurethane (TPU) fibers and a supramolecular ionic biopolymer. The interlocked binary assembly enables skin-like softness, high stretchability, and strain-adaptive stiffening through a matrix-to-scaffold stress transfer. The Bouligand structure contributes to superhigh fracture toughness (101.6 kJ m -2 ) and fatigue resistance (4937 J m -2 ) via mechanical toughening by interlayer slipping and twisted crack propagation path. Besides, the STFSI elastomer is self-healable through a "bridging" method and environment-tolerant (-20 °C, strong acid/alkali, saltwater). To demonstrate the versatile structural and sensing applications, we showcase a safety cushion with efficient damping and suppressed rebounding, and a robotic sensor with excellent fatigue crack tolerance and instant sensation recovery upon cutting-off damage. Our presented synthetic strategy is generalizable to other fiber-reinforced tough polymers for applications involving demanding mechanical/environmental conditions., (© 2024 Wiley-VCH GmbH.)

CO 2 electroreduction into liquid fuels is of broad interest and benefits reducing the energy crisis and environment burdens. CuS has been reported to be a desirable candidate for CO 2 electroreduction into formate; however, its formate selectivity and stability are still far from the demands of practical application. Herein, we report CuS nanoparticles exhibiting good Faradaic efficiency of formate (about 98 %) in CO 2 electroreduction and its deactivation mechanism during the reaction. The deactivation of CuS was found to be associated with the reconstruction and S loss of CuS, which deteriorates the Faradaic efficiency of formate. Combined with ionic and gas analyses, the S atom in CuS was lost in the form of H 2 S, SO 2 , and SO 4 2- , followed by the reconstruction of CuS into copper oxides. Such a catalyst reconstruction facilitates electroreductions of CO 2 and H 2 O, respectively, into CO and H 2 , etc., resulting in the degradation of catalytical performance of CO 2 electroreduction into formate. This work reveals the important role of S loss and reconstruction of metal sulfide catalysts during the electroreduction reaction, which may benefit the further development of CuS-based electro-catalyst for CO 2 electroreduction., (© 2023 Wiley-VCH GmbH.)

Bioelectric electrodes with low modulus and high adhesion have been intensively pursued, as they afford conformal and strong bonding at skin-electrode interface to improve the fidelity and stability of electrophysiological signals. However, during detachment, tough adhesion can cause pain or skin allergy; worse still, the soft electrodes can suffer damage due to excessive stretch/torsion, hampering long-term, dynamic, and multiple uses. Herein, a bioelectric electrode is proposed by transferring silver nanowires (AgNWs) network to the surface of bistable adhesive polymer (BAP). The phase transition temperature of BAP is tuned to be slightly below skin temperature at 30 °C. Triggered by skin heat, the BAP electrode achieves low modulus and high adhesion within seconds, allowing robust skin-electrode interface under dry, wet, and body-moving conditions. Ice bag treatment can dramatically stiffen the electrode and reduce the adhesion, which allows painless detachment and avoids electrode damage. Meanwhile, the AgNWs network with biaxial wrinkled microstructure remarkably promotes the electro-mechanical stability of the BAP electrode. The BAP electrode successfully combines long-term (7 days) and dynamic (body movements, sweat, underwater) stability, reusability (at least ten times), and minimized skin irritation during electrophysiological monitoring. The high signal-to-noise ratio and dynamic stability are demonstrated in the application of piano-playing training., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Electricity generation and chemical productions are both critically important for the sustainable development of modern civilization. Here, a novel bifunctional Zn-organic battery has been established for the concurrent enhanced electricity output and semi-hydrogenations of a series of biomass aldehyderivatives, for the high value-added chemical syntheses. Among them, the typical Zn-furfural (FF) battery equipped with Cu foil-supported edge-enriched Cu nanosheets as cathodic electrocatalyst (Cu NS/Cu foil), provides a maximum current density and power density of 14.6 mA cm -2 and 2.00 mW cm -2 , respectively, and in the meantime, produces high value product, furfural alcohol (FAL). The Cu NS/Cu foil catalyst exhibits excellent electrocatalytic performance of ≈93.5 % conversion ratio and ≈93.1 % selectivity for FF semi-hydrogenation at a low potential of -1.1 V vs. Ag/AgCl by using H 2 O as H source, and shows impressive performance for various biomass aldehyderivatives semi-hydrogenation., (© 2023 Wiley-VCH GmbH.)

The spontaneous reaction between Zn and H 2 O is of critical importance and could plausibly be used to produce H 2 gas, especially under neutral conditions. However, this reaction has long been overlooked owing to its sluggish kinetics and Zn consumption. Herein, a unique self-co-electrolysis system (SCES) is reported, which uses a Zn anode, a CoP-based catalytic cathode, and a neutral phosphate buffer solution (PBS) as the electrolyte. In this SCES, Zn is not only a sacrificial anode but also an important precursor of high-value-added NaZnPO 4 . Additionally, the composition and phase structure of NaZnPO 4 can be well regulated. In this study, a high-performance N,Cu-CoP/carbon cloth (CC) catalyst is synthesized to catalyze the cathodic hydrogen evolution reaction (HER) at an especially low overpotential of 64.7 mV at 10 mA cm - 2 . H 2 gas (13.7 mL cm - 2 h - 1 ) and NaZnPO 4 (3.73 mg cm - 2 h - 1 ) are obtained at the cathode and anode, respectively, in the N,Cu-CoP/CC||Zn SCES spontaneously. Moreover, the SCES has a favorable open-circuit voltage (OCV) of 0.79 V and a maximum power density of 1.83 mW cm - 2 . Density functional theory (DFT) calculations are performed to elucidate the electronic structure and HER catalytic mechanism of the N and Cu co-doped CoP catalysts., (© 2022 Wiley-VCH GmbH.)

The innate immune system plays a key role in protecting the human body from tumors, which, unfortunately, is largely counteracted by their immune-suppression function. Such an immune suppression has been reported to be induced by the immunosuppressive microenvironment, including the exhausted cytotoxic T lymphocytes (CTLs) and tumor-promoting M2-polarized macrophages. Here, a novel tumor-immunotherapeutic modality based on the nanocatalytic innate immunity activation by tumor-specific mitochondrial DNA (mtDNA) oxidative damage is proposed. In detail, a nanocatalytic medicine, Fe 2+ -Ru 2+ -loaded mesoporous silica nanoparticle named as MSN-Ru 2+ /Fe 2+ (MRF), is constructed to induce oxidative damage in the mtDNA of tumor cells. Such an oxidative mtDNA is able to escape from the tumor cells and acts as an immunogenic damage-associated molecular pattern to M1-polarize tumor-associated macrophages (TAMs), resulting in the reactivated immunoresponse of macrophages against cancer cells, and the subsequent inflammatory response of innate immunity. Most importantly, the treatment strategy based on regulating the innate immune response of TAMs not only stops the primary tumor progression, but also almost completely inhibits the growth of distant tumors in the periods of treatments., (© 2021 Wiley-VCH GmbH.)

The electrochemical conversion of carbon dioxide into energy-carrying compounds or value-added chemicals is of great significance for diminishing the greenhouse effect and the efficient utilization of carbon-dioxide emissions, but it suffers from the kinetically sluggish anodic oxygen evolution reaction (OER) and its less value-added production of O 2 . We report a general strategy for efficient formic-acid synthesis by a concurrent cathodic CO 2 reduction and anodic partial methanol-oxidation reaction (MOR) using mesoporous SnO 2 grown on carbon cloth (mSnO 2 /CC) and CuO nanosheets grown on copper foam (CuONS/CF) as cathodic and anodic catalysts, respectively. Anodic CuONS/CF enables an extremely lowered potential of 1.47 V vs. RHE (100 mA cm -2 ), featuring a significantly enhanced electro-activity in comparison to the OER. The cathodic mSnO 2 /CC shows a rather high Faraday efficiency of 81 % at 0.7 V vs. RHE for formic-acid production from CO 2 . The established electrolyzer equipped with CuONS/CF at the anode and mSnO 2 /CC at the cathode requires a considerably low cell voltage of 0.93 V at 10 mA cm -2 for formic-acid production at both sides., (© 2020 Wiley-VCH GmbH.)

Pancreatic ductal adenocarcinoma (PDAC) is one of the deadliest malignant tumors with extremely poor prognosis due to the later stage diagnosis when surgical resection is no longer applicable. Alternatively, the traditional gene therapy which drives pancreatic cancer cells into an inactive state and inhibiting the proliferation and metastasis, presents potentials to safely inhibit pancreatic cancer progression, but unfortunately has received limited success to date. Here, an efficient gene therapy of pancreatic cancer is shown via a peptide nucleic acid (PNA)-loaded layered double hydroxides (LDHs) nanoplatform. Compared with the traditional DNA- or RNA-based gene therapies, the gene therapy using PNA features great advantages in recognizing and hybridizing with the target mutant sequences to form PNA-DNA hybrids with significantly enhanced stability due to the absence of electrostatic repulsion, and the constrained flexibility of the polyamide backbone. Moreover, ultrasmall LDHs are engineered to load PNA and the obtained PNA-loaded LDH platform (LDHs/PNA) is capable of efficiently and selectively targeting the intranuclear mutant sequences thanks to the proton sponge effect. Treatments with LDHs/PNA demonstrate markedly inhibited growth of pancreatic cancer xenografts via a cancer cell proliferation suppression mechanism. The results demonstrate the great potentials of LDHs/PNA as a highly promising gene therapy agent for PDAC., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Mg batteries have the advantages of resource abundance, high volumetric energy density, and dendrite-free plating/stripping of Mg anodes. However the injection of highly polar Mg 2+ cannot maintain the structural integrity of intercalation-type cathodes even for open framework prototypes. The lack of high-voltage electrolytes and sluggish Mg 2+ diffusion in lattices or through interfaces also limit the energy density of Mg batteries. Mg-S system based on moderate-voltage conversion electrochemistry appears to be a promising solution to high-energy Mg batteries. However, it still suffers from poor capacity and cycling performances so far. Here, a ZIF-67 derivative carbon framework codoped by N and Co atoms is proposed as effective S host for highly reversible Mg-S batteries even under high rates. The discharge capacity is as high as ≈600 mA h g -1 at 1 C during the first cycle, and it is still preserved at ≈400 mA h g -1 after at least 200 cycles. Under a much higher rate of 5 C, a capacity of 300-400 mA h g -1 is still achievable. Such a superior performance is unprecedented among Mg-S systems and benefits from multiple factors, including heterogeneous doping, Li-salt and Cl - addition, charge mode, and cut-off capacity, as well as separator decoration, which enable the mitigation of electrode passivation and polysulfide loss., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The introduction of active transition metal sites (TMSs) in carbon enables the synthesis of noble-metal-free electrocatalysts for clean energy conversion applications; however, there are often multiple existing forms of TMSs, which are of different natures and catalytic models. Regulating the evolution of distinctive TMSs is highly desirable but remains challenging to date. Anions, as essential elements involved in the synthesis, have been totally neglected previously in the construction of TMSs. Herein, the effects of anions on the creation of different types of TMSs are investigated for the first time. It is found that the active cobalt-nitrogen sites tend to be selectively constructed on the surface of N-doped carbon by using chloride, while metallic cobalt nanoparticles encased in protective graphite layers are the dominant forms of cobalt species with nitrate ions. The obtained catalysts demonstrate cobalt-sites-dependent activity for oxygen reduction reaction and hydrogen evolution reaction in acidic media. The remarkably enhanced catalytic activities approaching that of benchmark Pt/C in an acidic medium have been obtained on the catalyst dominated with cobalt-nitrogen sites, confirmed by the advanced spectroscopic characterization. This finding demonstrates a general paradigm of anion-regulated evolution of distinctive TMSs, providing a new pathway for enhancing performances of various targeted reactions related with TMSs., (© 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A nitrogen-doped vesicle-like porous carbon with well-integrated dual iron-based catalytic sites was developed through direct pyrolysis of inexpensive and abundant precursors. Benefiting from the mesoporous structures with synchronous construction of Fe-N x and Fe/Fe 3 C@NC sites, the optimized catalyst exhibited outstanding performance for the oxygen reduction reaction (ORR) in alkaline media, even superior to the commercial Pt/C catalyst. Detailed characterizations revealed that Fe/Fe 3 C@NC sites can make major catalytic contributions in basic media, whereas the Fe-N x sites were found to play an indispensable role for ORR in acidic media., (© 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Although Pt/C catalysts show relatively high activities for the oxygen reduction reaction (ORR) and great potential for use in polymer electrolyte membrane fuel cells, the large amount of Pt required and the poor stability of Pt/C-based catalysts remain big challenges. Herein, mesoporous Na4 Ge9 O20 micro-crystals have been successfully synthesized to serve as a new kind of electrocatalyst support owing to its special structural characteristics and high structural stability. After loading a low amount of Pt (5 wt %) nanoparticles of 2-5 nm in diameter, the obtained mesoporous Pt/Na4 Ge9 O20 composite shows not only high electrocatalytic activity for ORR in both acidic and alkaline electrolyte media, which are comparable to those of conventional 20 wt % Pt/C, but also remarkably enhanced Pt mass-specified ORR current density and durability. Synergetic catalytic effects between loaded Pt and the support for the ORR activity has been proposed., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Organic-inorganic hybrid materials aiming to combine the individual advantages of organic and inorganic components while overcoming their intrinsic drawbacks have shown great potential for future applications in broad fields. In particular, the integration of functional organic fragments into the framework of mesoporous silica to fabricate mesoporous organosilica materials has attracted great attention in the scientific community for decades. The development of such mesoporous organosilica materials has shifted from bulk materials to nanosized mesoporous organosilica nanoparticles (designated as MONs, in comparison with traditional mesoporous silica nanoparticles (MSNs)) and corresponding applications in nanoscience and nanotechnology. In this comprehensive review, the state-of-art progress of this important hybrid nanomaterial family is summarized, focusing on the structure/composition-performance relationship of MONs of well-defined morphology, nanostructure, and nanoparticulate dimension. The synthetic strategies and the corresponding mechanisms for the design and construction of MONs with varied morphologies, compositions, nanostructures, and functionalities are overviewed initially. Then, the following part specifically concentrates on their broad spectrum of applications in nanotechnology, mainly in nanomedicine, nanocatalysis, and nanofabrication. Finally, some critical issues, presenting challenges and the future development of MONs regarding the rational synthesis and applications in nanotechnology are summarized and discussed. It is highly expected that such a unique molecularly organic-inorganic nanohybrid family will find practical applications in nanotechnology, and promote the advances of this discipline regarding hybrid chemistry and materials., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A stability-difference-selective bond-breakage strategy for the fabrication of largepore-sized hollow mesoporous organosilica nanoparticles (HMONs) is successfully developed. Moreover, surfacefunctionalized HMONs are successfully constructed to simultaneously deliver P-gp modulator siRNA and anticancer drug doxorubicin to reverse the multidrug resistance of cancer cells., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Metallic glasses and cancer theranostics are emerging fields that do not seem to be related to each other. Herein, we report the facile synthesis of amorphous iron nanoparticles (AFeNPs) and their superior physicochemical properties compared to their crystalline counterpart, iron nanocrystals (FeNCs). The AFeNPs can be used for cancer theranostics by inducing a Fenton reaction in the tumor by taking advantage of the mild acidity and the overproduced H2 O2 in a tumor microenvironment: Ionization of the AFeNPs enables on-demand ferrous ion release in the tumor, and subsequent H2 O2 disproportionation leads to efficient (.)OH generation. The endogenous stimuli-responsive (.)OH generation in the presence AFeNPs enables a highly specific cancer therapy without the need for external energy input., (© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The biological mechanisms of nuclear-targeting mesoporous silica nanoparticles (MSNs)-based DDSs (DOX@NT-MSNs) in overcoming multidrug resistance of cancer cells are studied. It is interesting to find for the first time that DOX@NT-MSNs down-regulate the expression of apoptosis suppressor genes and inhibit DNA repair process by disturbing the p53 pathway., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Local hypoxia in tumors is an undesirable consequence of photodynamic therapy (PDT), which will lead to greatly reduced effectiveness of this therapy. Bioreductive pro-drugs that can be activated at low-oxygen conditions will be highly cytotoxic under hypoxia in tumors. Based on this principle, double silica-shelled upconversion nanoparticles (UCNPs) nanostructure capable of co-delivering photosensitizer (PS) molecules and a bioreductive pro-drug (tirapazamine, TPZ) were designed (TPZ-UC/PS), with which a synergetic tumor therapeutic effect has been achieved first by UC-based (UC-) PDT under normal oxygen environment, immediately followed by the induced cytotoxicity of activated TPZ when oxygen is depleted by UC-PDT. Treatment with TPZ-UC/PS plus NIR laser resulted in a remarkably suppressed tumor growth as compared to UC-PDT alone, implying that the delivered TPZ has a profound effect on treatment outcomes for the much-enhanced cytotoxicity of TPZ under PDT-induced hypoxia., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Strong oxygen dependence and limited penetration depth are the two major challenges facing the clinical application of photodynamic therapy (PDT). In contrast, ionizing radiation is too penetrative and often leads to inefficient radiotherapy (RT) in the clinic because of the lack of effective energy accumulation in the tumor region. Inspired by the complementary advantages of PDT and RT, we present herein the integration of a scintillator and a semiconductor as an ionizing-radiation-induced PDT agent, achieving synchronous radiotherapy and depth-insensitive PDT with diminished oxygen dependence. In the core-shell Ce(III)-doped LiYF4@SiO2@ZnO structure, the downconverted ultraviolet fluorescence from the Ce(III)-doped LiYF4 nanoscintillator under ionizing irradiation enables the generation of electron-hole (e(-)-h(+)) pairs in ZnO nanoparticles, giving rise to the formation of biotoxic hydroxyl radicals. This process is analogous to a type I PDT process for enhanced antitumor therapeutic efficacy., (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A novel micelle/precursor co-templating assembly strategy is successfully developed to synthesize large-pore ultrasmall mesoporous organosilica nanoparticles (MONs). Furthermore, elaborately designed MONs with a cell-penetrating peptide (TAT) (MONs-PTAT) are constructed for highly efficient intranuclear gene delivery. They exhibit a high loading capacity, improved protection for the loaded gene, and enhanced transfection efficiencies of EGFP plasmid (pEGFP)., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The successful cancer eradication in a noninvasive manner is the ultimate objective in the fight against cancer. As a "bloodless scalpel," high-intensity focused ultrasound (HIFU) is regarded as one of the most promising and representative noninvasive therapeutic modalities for cancer surgery. However, large-scale clinical applications of HIFU are still in their infancy because of critical efficiency and safety issues which remain to be solved. Fortunately, recently developed nanobiotechnology provides an alternative efficient approach to improve such important issues in HIFU, especially for cancer therapy. This Research News presents the very recent exciting progresses on the elaborate design and fabrication of organic, inorganic, and organic/inorganic hybrid nanoparticles for enhancing the HIFU ablation efficiency against tumor tissues. It is highly expected that this Research News can arouse more extensive research enthusiasm on the development of functional nanomaterials for highly efficient HIFU-based synergistic therapy, which will give a promising noninvasive therapeutic modality for the successful cancer therapy with minimal damage to surrounding normal tissues, due to the noninvasive and site-specific therapeutic features of HIFU., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Mesoporous silica nanoparticles functionalized with peptides are developed for sequential drug delivery. The RGD peptide is used for vasculature/cell membrane targeting and the TAT peptide for nuclear targeting. Using this delivery strategy, a tumor in a murine xenograft model is successfully regressed., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Insufficient or excess drug doses, due to unknown actual drug concentrations at the focus, are one of the main causes of chemotherapy failure for cancers. In this regard, the real-time monitoring of the release of anticancer drugs from nanoparticle drug delivery systems is of crucial importance, but it remains a critical and unsolved challenge. Herein, we report the proposal and development of a novel concept of real-time monitoring of NIR-triggered drug release in vitro and in vivo by using simultaneous upconverted luminescence (UCL) and magnetic resonance (MR) imaging. Such a monitoring strategy features the high sensitivity of UCL and the high-resolution, noninvasiveness, and tissue-depth-independence of MR imaging. The dual-mode real-time and quantitative monitoring of drug release can be applied to determine online the drug concentrations in vivo in the tissue regions of interest and, therefore, to avoid insufficient or excess drug dosings., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

In the anti-cancer war, there are three main obstacles resulting in high mortality and recurrence rate of cancers: the severe toxic side effect of anti-cancer drugs to normal tissues due to the lack of tumor-selectivity, the multi-drug resistance (MDR) to free chemotherapeutic drugs and the deadly metastases of cancer cells. The development of state-of-art nanomedicines based on mesoporous silica nanoparticles (MSNs) is expected to overcome the above three main obstacles. In the view of the fast development of anti-cancer strategy, this review highlights the most recent advances of MSN anti-cancer nanomedicines in enhancing chemotherapeutic efficacy, overcoming the MDR and inhibiting metastasis. Furthermore, we give an outlook of the future development of MSNs-based anti-cancer nanomedicines, and propose several innovative and forward-looking anti-cancer strategies, including tumor tissue-cell-nuclear successionally targeted drug delivery strategy, tumor cell-selective nuclear-targeted drug delivery strategy, multi-targeting and multi-drug strategy, chemo-/radio-/photodynamic-/ultrasound-/thermo-combined multi-modal therapy by virtue of functionalized hollow/rattle-structured MSNs., (© 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Dual-mesoporous ZSM-5 zeolite with highly b axis oriented large mesopores was synthesized by using nonionic copolymer F127 and cationic surfactant CTAB as co-templates. The product contains two types of mesopores--smaller wormlike ones of 3.3 nm in size and highly oriented larger ones of 30-50 nm in diameter along the b axis--and both of them interpenetrate throughout the zeolite crystals and interconnect with zeolite microporosity. The dual-mesoporous zeolite exhibits excellent catalytic performance in the condensation of benzaldehyde with ethanol and greater than 99 % selectivity for benzoin ethyl ether at room temperature, which can be ascribed to the zeolite lattice structure offering catalytically active sites and the hierarchical and oriented mesoporous structure providing fast access of reactants to these sites in the catalytic reaction. The excellent recyclability and high catalytic stability of the catalyst suggest prospective applications of such unique mesoporous zeolites in the chemical industry., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The remarkable progress of nanotechnology and its application in biomedicine have greatly expanded the ranges and types of biomaterials from traditional organic material-based nanoparticles (NPs) to inorganic biomaterials or organic/inorganic hybrid nanocomposites due to the unprecedented advantages of the engineered inorganic material-based NPs. Colloidal mesoporous silica NPs (MSNs), one of the most representative and well-established inorganic materials, have been promoted into biology and medicine, and shifted from extensive in vitro research towards preliminary in vivo assays in small-animal disease models. In this comprehensive review, the recent progresses in chemical design and engineering of MSNs-based biomaterials for in vivo biomedical applications has been detailed and overviewed. Due to the intrinsic structural characteristics of elaborately designed MSNs such as large surface area, high pore volume and easy chemical functionalization, they have been extensively investigated for therapeutic, diagnostic and theranostic (concurrent diagnosis and therapy) purposes, especially in oncology. Systematic in vivo bio-safety evaluations of MSNs have revealed the evidences that the in vivo bio-behaviors of MSNs are strongly related to their preparation prodecures, particle sizes, geometries, surface chemistries, dosing parameters and even administration routes. In vivo pharmacokinetics and pharmacodynamics further demonstrated the effectiveness of MSNs as the passively and/or actively targeted drug delivery systems (DDSs) for cancer chemotherapy. Especially, the advance of nano-synthetic chemistry enables the production of composite MSNs for advanced in vivo therapeutic purposes such as gene delivery, stimuli-responsive drug release, photothermal therapy, photodynamic therapy, ultrasound therapy, or anti-bacteria in tissue engineering, or as the contrast agents for biological and diagnostic imaging. Additionally, the critical issues and potential challenges related to the chemical design/synthesis of MSNs-based "magic bullet" by advanced nano-synthetic chemistry and in vivo evaluation have been discussed to highlight the issues scientists face in promoting the translation of MSNs-based DDSs into clinical trials., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

A meostructured WO(3)/C composite with crystalline framework and high electric conductivity has been synthesized by a new in situ carbonization-replication route using the block copolymer (poly(ethylene glycol)-block-poly(propylene glycol)-block-poly(ethylene glycol)) present in situ in the pore channels of mesoporous silica template as carbon source. X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, thermogravimetry differential thermal analysis, and N(2) adsorption techniques were adopted for the structural characterization. Cyclic voltammetry, chronoamperometry, and single-cell test for hydrogen electrochemical oxidation were adopted to characterize the electrochemical activities of the mesoporous WO(3)/C composite. The carbon content and consequent electric conductivity of these high-surface-area (108-130 m(2) g(-1)) mesostructured WO(3)/C composite materials can be tuned by variation of the duration of heat treatment, and the composites exhibited high and stable electrochemical catalytic activity. The single-cell test results indicated that the mesostructured WO(3)/C composites showed clear electrochemical catalytic activity toward hydrogen oxidation at 25 °C, which makes them potential non-precious-metal anode catalysts in proton exchange membrane fuel cell., (Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Blackened catalyst: Zeolites with large external surface area and mesopore volume were synthesized by a one-pot templating strategy, in which the crystallization proceeded concurrently with in situ carbonization templating to produce a mesoporous structure. The hierarchical materials exhibited superior catalytic performance over conventional zeolites in Friedel-Crafts acylation of anisole., (Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Here we report the design and controlled synthesis of monodisperse and precisely size-controllable UCNP@mSiO(2) nanocomposites smaller than 50 nm by directly coating a mesoporous silica shell (mSiO(2)) on upconversion nanocrystals NaYF(4):Tm/Yb/Gd (UCNPs), which can be used as near-infrared fluorescence and magnetic resonance imaging (MRI) agents and a platform for drug delivery as well. Some key steps such as transferring hydrophobic UCNPs to the water phase by using cetyltrimethylammonium bromide (CTAB), removal of the excess amount of CTAB, and temperature-controlled ultrasonication treatment should be adopted and carefully monitored to obtain uniform upconversion core/mesoporous silica shell nanocomposites. The excellent performance of the core-shell-structured nanocomposite in near-infrared fluorescence and magnetic resonance imaging was also demonstrated., (Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

By kinetic control over the zeolite seed formation, we report the direct fabrication of hierarchical mesoporous zeolites using hexadecyl trimethyl ammonium bromide (CTAB) as the soft template in a conventional solution route. Nanometer-sized, subnanocrystal-type zeolite seeds with a high degree of polymerization are essential to prevent the formation of a separate amorphous mesoporous phase and the phase separation between the mesophase and zeolite crystals in the presence of CTAB and a certain amount of ethanol. The mechanisms for the formation of hierarchically porous zeolites in the solution process, including the effect of mother liquid aging, formation of subnanocrystal zeolite seeds and their self-assembly effect with CTAB, and the role of ethanol are proposed and discussed in detail. The prepared mesoporous ZSM-5 zeolite showed much higher catalytic activity than conventional counterparts for aldol condensations involving large molecules, especially in the synthesis of vesidryl., (Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The in vivo biodistribution and urinary excretion of spherical mesoporous silica nanoparticles (MSNs) are evaluated by tail-vein injection in ICR mice, and the effects of the particle size and PEGylation are investigated. The results indicate that both MSNs and PEGylated MSNs of different particle sizes (80-360 nm) distribute mainly in the liver and spleen, a minority of them in the lungs, and a few in the kidney and heart. The PEGylated MSNs of smaller particle size escape more easily from capture by liver, spleen, and lung tissues, possess longer blood-circulation lifetime, and are more slowly biodegraded and correspondingly have a lower excreted amount of degradation products in the urine. Neither MSNs nor PEGylated MSNs cause tissue toxicity after 1 month in vivo., (Copyright © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

In the context of revealing interfacial effects on ion conduction, thin films are extremely worthwhile due to defined geometry. Of particular interest are heterostructures as they offer symmetric boundary conditions and a high density of hetero-interfaces. The recent progress in this field is reviewed. Materials classes under concern include halides and oxides, and refer to various degrees of disorder and different mobilities. Even though in its infancy, the field of ionic heterostructures is already characterized by a variety of results of fundamental importance and of technological relevance., (Copyright © 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)