Publications by authors named "An-Wu Xu"

Cadmium sulfide (CdS) based heterojunctions, including type-II, Z-scheme, and S-scheme systems emerged as promising materials for augmenting photocatalytic hydrogen (H) generation from water splitting. This review offers an exclusive highlight of their fundamental principles, synthesis routes, charge transfer mechanisms, and performance properties in improving H production. We overview the crucial roles of Type-II heterojunctions in enhancing charge separation, Z-scheme heterojunctions in promoting redox potentials to reduce electron-hole (e/h) pairs recombination, and S-scheme heterojunctions in combining the merits of both type-II and Z-scheme frameworks to obtain highly efficient H production.

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In recent years, graphitic carbon nitride (g-CN) has attracted considerable attention because it includes earth-abundant carbon and nitrogen elements and exhibits good chemical and thermal stability owing to the strong covalent interaction in its conjugated layer structure. However, bulk g-CN has some disadvantages of low specific surface area, poor light absorption, rapid recombination of photogenerated charge carriers, and insufficient active sites, which hinder its practical applications. In this study, we design and synthesize potassium single-atom (K SAs)-doped g-CN porous nanosheets (CM-K, where X represents the mass of KHP added) via supramolecular self-assembling and chemical cross-linking copolymerization strategies.

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This study presents a green and practical visible-light-induced photosensitizer-free decarbonylative Minisci-type reaction using aldehydes as alkyl radical precursors. The photocatalytic system exhibits a broad substrate scope and synthetically useful yields. Mechanistic experiments revealed that alkyl radicals could be generated through auto-oxidation of aldehydes under irradiation, which is a mild and effective method for achieving late-stage functionalization of N-heteroarenes.

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Inspired by the two kinds of naturally occurring peroxidases (POD) with vanadium or heme (iron)-based active catalytic centers, we have developed a dual metal-based nanozyme with dual V and Fe-based active catalytic centers. Co-doping of graphene with heteroatoms has a synergistic effect on the catalytic properties of the nanomaterial as the distances of migration of the substrates drastically reduce. However, a few studies have reported the codoping of heterometallic elements in the graphene structure due to the complexity of the synthesis procedures.

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Chemotherapy, as one main strategy to relieve tumor progression, has a weak effect on triple-negative breast cancer (TNBC) chest wall metastasis. The development of near-infrared (NIR) light-responsive nanomaterials for chemodynamic therapy (CDT) and photothermal therapy (PTT) is a promising platform but still challenging in biomedicine. This study reports a peroxidase mimicking nanozyme (Fe-N-C SAzyme) against TNBC by CDT and PTT.

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The rational design and fabrication of high-performance and durable bifunctional non-noble-metal electrocatalysts for both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are still a great challenge in the practical applications of rechargeable zinc-air (Zn-air) batteries. Herein, we report a simple yet robust route to synthesize cobalt nanoparticles rooted in the hierarchically hollow nitrogen-doped carbon frameworks (Co@HNCs). This strategy employs the pyrolysis of nanostructured hollow Co-based metal-organic framework (ZIF-67) precursors produced by selective linker cleaving with pyrazino(2,3-)(1,10)phenanthroline-2,3-dicarboxylic acid molecules (HPPDA).

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Regulating the catalytic pathways of single-atom sites in single atom catalysts (SACs) is an exciting debate at the moment, which has redirected the research towards understanding and modifying the single-atom catalytic sites through various strategies including altering the coordination environment of single atom for desirable outcomes as well as increasing their number. One useful aspect concerning the tunability of the catalytic pathways of SACs, which has been overlooked, is the oxidation state dynamics of the single atoms. In this study, iron single-atoms (FeSA) with variable oxidation states, dependent on the precursors, are harnessed inside a nitrogen-rich functionalized carbon quantum dots (CQDs) matrix via a facile one-step and low-temperature synthesis process.

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Exploration of versatile nanoplatforms within one single nanostructure for multidisciplinary treatment modalities, especially achieving a synergistic therapeutic efficacy of combinational gene/photothermal cancer therapy is still a great challenge in biomedicine and nanotechnology. In this study, a unique photothermal nanocarrier has successfully been designed and developed for a combination of gene therapy (GT) and photothermal therapy (PTT) of cancer cells. Surface-engineered iron oxides (α-FeO) nanoparticles (NPs) with poly(3,4-ethylenedioxythiophene) (PEDOT) polymer coatings are synthesized using a one-pot oxidative polymerization method.

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A facile and large-scale construction of robust and inexpensive trifunctional self-supporting electrodes for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in metal-air batteries and water splitting is crucial but remains challenging. Herein, we report a direct and up-scalable all-solid-phase strategy for the synthesis of a porous three-dimensional electrode consisting of cobalt nanoparticles wrapped in nitrogen-doped carbon tubes (Co/N-CNTs), which are in situ planted onto the surface of a cobalt foam. The resultant Co/N-CNTs can directly serve as a self-supporting and adhesive-free electrode with excellent and durable catalytic performances for the ORR, OER and HER.

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Graphene oxide (GO) has recently been highlighted as a promising multipurpose two-dimensional material. However, free-standing graphene oxide films suffer from poor strength and flexibility, which limits scaling-up of production and lifetime structural robustness in applications. Inspired by the relationship between the organic and inorganic components of the hierarchical structure of nacre found in mollusk shells, we have fabricated self-assembled, layered graphene-based composite films.

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Exploring a combined phototherapeutic strategy to overcome the limitations of a single mode therapy and inducing high anticancer efficiency is highly promising for precision cancer nanomedicine. However, a single-wavelength laser activates dual photothermal/photodynamic therapy (PTT/PDT) treatment is still a formidable challenge. Herein, we strategically design and fabricate a multifunctional theranostic nanosystem based on chlorin e6-functionalized polydopamine (PDA) coated prussian blue/manganese dioxide nanoparticles (PB-MnO@PDA-Ce6 NPs).

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Development of near infrared (NIR) light-responsive nanomaterials for high performance multimodal phototherapy within a single nanoplatform is still challenging in technology and biomedicine. Herein, a new phototherapeutic nanoagent based on FDA-approved Prussian blue (PB) functionalized oxygen-deficient molybdenum oxide nanoparticles (MoO NPs) is strategically designed and synthesized by a facile one-pot size/morphology-controlled process. The as-prepared PB-MoO nanocomposites (NCs) with a uniform particle size of ∼90 nm and high water dispersibility exhibited strong optical absorption in the first biological window, which is induced by plasmon resonance in an oxygen-deficient MoO semiconductor.

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Inspired by the cascade reactions occurring in micro-organelles of living systems, we have developed a hybrid hydrogel, a nanozyme that mimics three key enzymes including peroxidase, superoxide dismutase, and catalase. The organic/inorganic nanostructured hydrogel constituting VO incorporated hexacyanoferrate Berlin green analogue complex (VOBG) is prepared by a simple one-step hydrothermal process, and its composition, structure, and properties are thoroughly investigated. Polyvinylpyrrolidone, a low-cost and biocompatible polymer, was utilized as a scaffold to increase the surface area and dispersion of the highly active catalytic centers of the nanozyme.

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The development of low-cost and highly efficient single-atom oxygen reduction catalysts to replace platinum for fuel cells and metal-air cells is highly desirable but remains challenging. Herein, we report the fabrication of isolated single-atom Fe anchored on porous nitrogen-doped carbon from the pyrolysis of a well-designed solely Fe-tetrapyridophenazine coordination complex. The N-rich bridging ligand, tetrapyridophenazine (tpphz) is first employed as a spatial isolation agent of Fe that suppresses its aggregation during high temperature pyrolysis, resulting in highly reactive and stable single-atom Fe ORR catalysts.

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Metal-organic framework (MOF)-based materials possess numerous attractive characteristics; however, the application of MOF-based photocatalysts in the area of visible-light photocatalytic H2 evolution is still in its infancy. Herein, we develop a series of novel UiO-66-NH2-based composites with embedded NiO nanoparticles via solvothermal treatment and subsequent calcination. Their characterizations demonstrate intimate lattice-level contacts between UiO-66-NH2 photocatalysts and NiO nanoparticles.

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In this study, we report a simple method to prepare nitrogen-doped graphene, with which a nitrogen-doped graphene/SnO2 composite was successfully fabricated and employed as a lithium battery anode. Electrochemical test results indicated that the as-prepared nitrogen-doped graphene/SnO2 electrode possesses high reversible capacity and outstanding charging and discharging capabilities, which would make it possible to meet the requirements for portable electronic devices in the future. These super electrochemical properties could benefit from the synergistic effect of SnO2 nanoparticles that contribute to the high capacity and nitrogen-doped graphene that could enhance the electroconductivity.

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Heteropolyacids (HPAs) are a class of polyoxometallates (POMs) with oxygen-rich surfaces. Herein, we have developed an Fe-containing heteropolyacid by cation-exchange and employed KFePW12O40 nanostructures for Fenton, photo-Fenton and enzyme-mimetic reactions. The as-prepared KFePW12O40 catalyst exhibits efficient degradation of Rhodamine B (RhB) via the photo-Fenton reaction.

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The design and development of highly efficient and long lifetime Pd-based catalysts for hydrogenation reactions have attracted significant research interest over the past few decades. Rational selection of supports for Pd loadings with strong metal-support interaction (SMSI) is beneficial for boosting catalytic activity and stability. In this context, we have developed a facile approach for uniformly immobilizing ultra-small Pd nanoparticles (NPs) with a clean surface on a PrO support by a hydrogen thermal reduction method.

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Heterogeneous catalytic hydrogenation reactions are of great importance to the petrochemical industry and fine chemical synthesis. Herein, we present the first example of gadolinium hydroxide (Gd(OH)) nanorods as a support for loading ultra-small Pd nanoparticles for hydrogenation reactions. Gd(OH) possesses a large number of hydroxyl groups on the surface, which act as an ideal support for good dispersion of Pd nanoparticles.

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Electrochemical water splitting is an important process to produce hydrogen and oxygen for energy storage and conversion devices. However, it is often restricted by the oxygen evolution reaction (OER) due to its sluggish kinetics. To overcome the problem, precious metal oxide-based electrocatalysts, such as RuO and IrO, are widely used.

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Efficient and durable oxygen evolution reaction (OER) catalysts are highly required for the cost-effective generation of clean energy from water splitting. For the first time, an integrated OER electrode based on one-step direct growth of metallic iron-nickel sulfide nanosheets on FeNi alloy foils (denoted as FeNi S /FeNi) is reported, and the origin of the enhanced OER activity is uncovered in combination with theoretical and experimental studies. The obtained FeNi S /FeNi electrode exhibits highly catalytic activity and long-term stability toward OER in strong alkaline solution, with a low overpotential of 282 mV at 10 mA cm and a small Tafel slope of 54 mV dec .

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Metal/support nanocatalysts consisting of various metals and metal oxides not only retain the basic properties of each component but also exhibit higher catalytic activity due to their synergistic effects. Herein, we report the creation of a highly efficient, long-lasting, and magnetic recyclable catalyst, composed of magnetic nickel (Ni) nanoparticles (NPs), active Pd NPs, and oxygen-deficient CeO support. These hybrid nanostructures composed of oxygen deficient CeO and active metal nanoparticles could effectively facilitate diffusion of reactant molecules and active site exposure that can dramatically accelerate the reaction rate.

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As the ever-growing demand for high-performance power sources, lithium-ion batteries with high storage capacities and outstanding rate performance have been widely considered as a promising storage device. In this work, starting with metal-organic frameworks, we have developed a facile approach to the synthesis of hybrid FeO/VO hollow microboxes via the process of hydrolysis and ion exchange and subsequent calcination. In the constructed architecture, the hollow structure provides an efficient lithium ion diffusion pathway and extra space to accommodate the volume expansion during the insertion and extraction of Li.

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We report a novel reversible color switching system based on one-pot hydrogenation/oxygenation reactions over Pd/CeO catalysts and fast interconversion of thionine (TH) and leuco thionine (LTH). Oxygen vacancies produced by Pd-catalyzed instant hydrogenation of CeO and strong metal-support interaction (SMSI) could lead to fast color switching.

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It is an ongoing challenge to fabricate nonprecious oxygen reduction reaction (ORR) catalysts that can be comparable to or exceed the efficiency of platinum. A highly active non-platinum self-supporting Fe-N/C catalyst has been developed through the pyrolysis of a new type of precursor of iron coordination complex, in which 1,4-bis(1H-1,3,7,8-tetraazacyclopenta(1)phenanthren-2-yl)benzene (btcpb) functions as a ligand complexing Fe(II) ions. The optimal catalyst pyrolyzed at 700 °C (Fe-N/C-700) shows the best ORR activity with a half-wave potential (E ) of 840 mV versus reversible hydrogen electrode (RHE) in 0.

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