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Photoactive colloidal motors whose motion can be controlled and even programed via external magnetic fields have significant potential in practical applications extending from biomedical fields to environmental remediation. Herein, we report a "three in one" strategy in a Co/Zn-TPM (3-trimethoxysilyl propyl methacrylate) bimetallic Janus colloidal micromotor (BMT-micromotor) which can be controlled by an optical field, chemical fuel, and magnetic field. The speed of the micromotors can be tuned by light intensity and with the concentration of the chemical fuel of H 2 O 2 , while it could be steered and programed through magnetic field due to the presence of Co in the bimetallic part. Finally, the BMT-micromotors were employed to effectively remove rubidium metal ions and organic dyes (methylene blue and rhodamine b). Benefited of excellent mobility, multiple active sites, and hierarchical morphology, the micromotors exhibit excellent adsorption capacity of 103 mg·g -1 to Rb metal ions and high photodegradation efficiency toward organic dyes in the presence of a lower concentration of H 2 O 2 . The experimental characterizations and DFT calculations confirmed the strong interaction of Rb metal ions on the surface of BMT-micromotors and the excellent decomposition of H 2 O 2 which enhanced the photodegradation process. We expect the combination of light and fuel sensitivity with magnetic controllability to unlock an excess of opportunities for the application of BMT-micromotors in water treatments.

The fate and effects of fluoroquinolone antibacterial (FQ) on the environment are important since there appears to be a surge in FQ resistance like enrofloxacin (ENR) in both environmental and clinical organisms. Numerous reports indicate that the sensing capabilities of these antibiotics need to be improved. Here, we have investigated the interaction of ENR with our synthesized pentacenequinone-modulated gadolinium-tin (GdSn-PQ) nanosheets and the formation of intermolecular interactions that caused the occurrence of aggregation-induced emission enhancement. The concept for designing hybrid metallic nanosheets comes from the unique features inherited from the parent organic precursor. Due to the distinct interaction between ENR and GdSn-PQ, the interstate conversion (ISC) between GdSn-PQ and ENR induces a significant wavelength shift in photoluminescence (PL), improving reliability, selectivity, and visibility compared to quenching- or AIEE-based methods without peak shifts, allowing for highly sensitive and visually detectable analyses. The fluorescence signal of GdSn-PQ exhibited a linear relationship ( R 2 = 0.9911), with the added ENR concentrations ranging from 5 to 90 nM, with a detection limit of 0.10 nM. We have demonstrated its potential and wide use in the detection of ENR in biological samples (human urine and blood serum) and environmental samples (tap water and seawater) with a recovery rate of 98- 108%. The current approach has demonstrated that the 2D GdSn-PQ nanosheet is a novel and powerful platform for future biological and environmental studies.

We have synthesized Pt 1 Zn 3 /ZnO, also termed 0.01 wt %Pt/ZnO-O 2 -H 2 , as a catalyst containing singly dispersed single-atom bimetallic sites, also called a catalyst of singly dispersed bimetallic sites or a catalyst of isolated single-atom bimetallic sites. Its catalytic activity in partial oxidation of methanol to hydrogen at 290 °C is found to be 2-3 orders of magnitude higher than that of Pt-Zn bimetallic nanoparticles supported on ZnO, 5.0 wt %Pt/ZnO-N 2 -H 2 . Selectivity for H 2 on Pt 1 Zn 3 /ZnO reaches 96%-100% at 290-330 °C, arising from the uniform coordination environment of single-atom Pt 1 in singly dispersed single-atom bimetallic sites, Pt 1 Zn 3 on 0.01 wt %Pt/ZnO-O 2 -H 2 , which is sharply different from various coordination environments of Pt atoms in coexisting Pt x Zn y ( x ≥ 0, y ≥ 0) sites on Pt-Zn bimetallic nanoparticles. Computational simulations attribute the extraordinary catalytic performance of Pt 1 Zn 3 /ZnO to the stronger adsorption of methanol and the lower activation barriers in O-H dissociation of CH 3 OH, C-H dissociations of CH 2 O to CO, and coupling of intermediate CO with atomic oxygen to form CO 2 on Pt 1 Zn 3 /ZnO as compared to those on Pt-Zn bimetallic nanoparticles. It demonstrates that anchoring uniform, isolated single-atom bimetallic sites , also called singly dispersed bimetallic sites on a nonmetallic support can create new catalysts for certain types of reactions with much higher activity and selectivity in contrast to bimetallic nanoparticle catalysts with coexisting, various metallic sites M x A y ( x ≥ 0, y ≥ 0). As these single-atom bimetallic sites are cationic and anchored on a nonmetallic support, the catalyst of singly dispersed single-atom bimetallic sites is different from a single-atom alloy nanoparticle catalyst. The critical role of the 0.01 wt %Pt in the extraordinary catalytic performance calls on fundamental studies of the profound role of a trace amount of a metal in heterogeneous catalysis.

Ammonia (NH 3 ) plays a vital role in industrial and agricultural development. The electrocatalytic nitrate reduction reaction (eNO 3 RR) is an effective method to produce NH 3 under environmental conditions but also requires considerably active and selective electrocatalysts. Herein, a copper foam was used as a conductive substrate for the electrode materials. Specifically, a Co metal-organic framework (Co-MOF) was in situ grown on the copper foam, etched, and calcined to form NiCoO 2 @Cu nanosheets, which were used as cathode electrodes for the eNO 3 RR. In 0.1 M Na 2 SO 4 with 0.1 M NaNO 3 electrolyte, NiCoO 2 @Cu nanosheets realized an NH 3 yield of 5940.73 μg h -1 cm -2 at -0.9 V vs reversible hydrogen electrode (RHE), with a Faradaic efficiency of 94.2% at -0.7 V vs RHE. After 33 h of the catalytic reaction, the selectivity of NH 3 -N increased to 99.7%. The excellent electrocatalytic performance of NiCoO 2 @Cu nanosheets was attributed to the apparent synergistic effect between the Ni atoms and the Co atoms of bimetallic materials. This study shows that the Ni doping of NiCoO 2 @Cu nanosheets effectively facilitated the adsorption of NO 3 - on NiCoO 2 @Cu, and it promoted the eNO 3 RR.

Conventional antibiotic-based treatment of bacterial infections remains one of the most difficult challenges in medicine because of the threat of multidrug resistance caused by indiscriminate abuse. To solve these problems, it is essential to develop an effective antibacterial agent that can be used at a small dose while minimizing the occurrence of multiple resistance. Metal-organic frameworks (MOFs), which are hyper-porous hybrid materials containing metal ions linked by organic ligands, have recently attracted attention because of their strong antibacterial activity through metal-ion release, unlike conventional antibiotics. In this study, we developed a photoactive MOF-derived cobalt-silver bimetallic nanocomposite (Ag@CoMOF) by simply depositing silver nanoparticles on a cobalt-based MOF through nanoscale galvanic replacement. The nanocomposite structure continuously releases antibacterial metal ions (i.e., Ag and Co ions) in the aqueous phase and exhibits a strong photothermal conversion effect of Ag nanoparticles, accompanied by a rapid temperature increase of 25-80 °C under near-infrared (NIR) irradiation. Using this MOF-based bimetallic nanocomposite, superior antibacterial activities were achieved by 22.1-fold for Escherichia coli and 18.3-fold for Bacillus subtilis enhanced inhibition of bacterial growth in a liquid culture environment compared with the generally used chemical antibiotics. In addition, we confirmed the synergistic enhancement of the antibacterial ability of the bimetallic nanocomposite induced by NIR-triggered photothermal heating and bacterial membrane disruption even when using a small amount of the nanocomposites. We envision that this novel antibacterial agent using MOF-based nanostructures will replace traditional antibiotics to circumvent multidrug resistance and present a new approach to antibiotic development.

The present research work facilitates a ligand-mediated effective strategy to achieve different morphological surface structures of bimetallic (Ni and Co) metal-organic frameworks (MOFs) by utilizing different types of organic ligands like terephthalic acid (BDC), 2-methylimidazole (2-Melm), and trimesic acid (BTC). Different morphological structures, rectangular-like nanosheets, petal-like nanosheets, and nanosheet-assembled flower-like spheres (NSFS) of NiCo MOFs, are confirmed from the structural characterization for ligands BDC, 2-Melm, and BTC, respectively. The basic characterization studies like scanning electron microscopy, X-ray diffraction, transmission electron microscopy, and Brunauer-Emmett-Teller revealed that the NiCo MOF prepared by using trimesic acid as the ligand (NiCo MOF_BTC) with a long organic linker exhibits a three-dimensional architecture of NSFS that possesses higher surface area and pore dimensions, which enables better ion kinetics. Also, the NiCo MOF_BTC delivered the highest capacity of 1471.4 C g -1 (and 408 mA h g -1 ) at 1 A g -1 current density, compared to the other prepared NiCo MOFs and already reported different NiCo MOF structures. High interaction of trimesic acid with the metal ions confirmed from ultraviolet-visible spectroscopy and X-ray photoelectron spectroscopy leads to a NSFS structure of NiCo MOF_BTC. For practical application, an asymmetric supercapacitor device (NiCo MOF_BTC//AC) is fabricated by taking NiCo MOF_BTC and activated carbon as the positive and negative electrode, respectively, where the PVA + KOH gel electrolyte serves as a separator as well as an electrolyte. The device delivered an outstanding energy density of 78.1 Wh kg -1 at a power density of 750 W kg -1 in an operating potential window of 1.5 V. In addition, it displays a long cycle life of 5000 cycles with only 12% decay of the initial specific capacitance. Therefore, these findings manifest the morphology control of MOFs by using different ligands and the mechanism behind the different morphologies that will provide an effective way to synthesize differently structured MOF materials for future energy-storage applications.

Bimetallic zeolitic imidazolate frameworks (ZIFs) containing two different metal ions can exhibit superior performances when applied in heterogeneous catalysis. Herein, we present a facile one-pot synthesis method for PdCo-ZIFs with various Pd/Co ratios, where Pd(II) ions are successfully incorporated into the Co node sites of the ZIF structure. The local structure of the bimetallic ZIFs was comprehensively investigated by pore-structure, X-ray absorption fine structure, and in situ CO adsorption Fourier transform infrared analyses. The results demonstrated that the framework comprises different coordination geometries of Co (tetrahedral) and Pd (square planar) ions connected by the benzimidazolate ligand. Notably, the inherently nonporous, 2D Co-ZIF structure was transformed into a hierarchical porous structure, and the PdCo-ZIFs exhibited a significantly increased concentration of defects and distorted Co sites. Based on these results, the catalytic performances of the synthesized ZIFs in the cycloaddition of CO 2 to epoxides were evaluated under a cocatalyst and solvent-free conditions. The PdCo-ZIFs exhibited significantly higher catalytic activity (maximum turnover frequency, TOF = 2501 h -1 ) than Co-ZIF (TOF = 65 h -1 ) and Pd-ZIF (no activity), which revealed that the undercoordinated Co sites with distorted structure are the active sites rather than the incorporated Pd ions. This study provides a facile one-pot method for synthesizing bimetallic ZIFs with mixed-coordination modes, hierarchical porous structures, and modified defect concentrations, which would expand the library of structurally diverse bimetallic ZIFs toward various applications.

Electrocatalytic reduction of CO 2 into valuable fuels and chemical feedstocks in a sustainable and environmentally friendly manner is an ideal way to mitigate climate change and environmental problems. Here, we fabricated a series of self-supporting Bi-Sb bimetallic nanoleaves on carbon paper (CP) by a facile electrodeposition method. The synergistic effect of Bi and Sb components and the change of the electronic structure lead to high formate selectivity and excellent stability in the electrochemical CO 2 reduction reaction (CO 2 RR). Specifically, the Bi-Sb/CP bimetallic electrode achieved a high Faradic efficiency (FE formate , 88.30%) at -0.9 V (vs RHE). The FE of formate remained above 80% in a broad potential range of -0.9 to -1.3 V (vs RHE), while FE CO was suppressed below 6%. Density functional theory calculations showed that Bi(012)-Sb reduced the adsorption energy of the *OCHO intermediate and promoted the mass transfer of charges. The optimally adsorbed *OCHO intermediate promoted formate production while inhibiting the CO product pathway, thereby enhancing the selectivity to formate synthesis. Moreover, the CO 2 RR performance was also investigated in a flow-cell system to evaluate its potential for industrial applications. The bimetallic Bi-Sb catalyst can maintain a steady current density of 160 mA/cm 2 at -1.2 V (vs RHE) for 25 h continuous electrolysis. Such excellent stability for formate generation in flow cells has rarely been reported in previous studies. This work offers new insights into the development of bimetallic self-supporting electrodes for CO 2 reduction.

Prussian blue analogs (PBAs) are regarded as promising cathode materials for sodium-ion batteries (SIBs), but most of them suffer from an incompatibility between capacity and structural stability. Herein, an innovative disodium ethylenediaminetetraacetate (Na 2 EDTA)-assisted hydrothermal method is proposed to synthesize monoclinic Fe-substituted Ni-rich PBA (H-PBA) cathodes for Na-ion storage. The as-designed H-PBA cathode combines the merits of the low strain of a Ni-based PBA framework and the enhanced capacity of N-Fe 3+ /Fe 2+ redox sites. It can achieve superior sodium-storage performance in terms of capacity, rate capability, and cycle stability. Moreover, ex situ measurements reveal that solid solution (2.0-3.0 V) and phase-transition (3.0-4.0 V) reactions occur during the charge/discharge process to allow almost 1.5 Na + storage in the H-PBA lattice. Meanwhile, the H-PBA//NaTi 2 (PO 4 ) 3 @C full cell also delivers remarkable electrochemical properties. Prospectively, this work would promote the practical application of SIBs in grid-scale electric energy storage.

The global ammonia yield is critical to the fertilizer industry as the global food demand is highly dependent on it, whereas, NH 3 is also a key chemical for pharmaceutical, textile, plastic, explosive, and dye-making industries. At present, the demand for NH 3 is fulfilled by the Haber-Bosch method, which consumes 1-3% of global energy and causes 0.5-1% CO 2 emission every year. To reduce emissions and improve energy efficiency, the electrochemical nitrogen gas reduction reaction (N 2 RR) has received much attention and support after the funding announcement by the U.S. Department of Energy. In this work, we have created hollow CuAu nanoboxes with Cu-rich inner walls to improve the NH 3 Faradaic efficiency in N 2 RR. These beveled nanoboxes are produced in different degrees of corner and edge etching, which produces both polyhedral and concave structures. In N 2 RR, the binary CuAu nanoboxes enhanced NH 3 production compared to individual Au and Cu nanocubes. The results of DFT calculations suggest the Cu-rich inner walls in the hollow beveled CuAu nanoboxes play a major role in their performance by reducing the free energy Δ G *NNH for the potential-determining step to form *NNH (* + N 2 (g) + H + + e - → *NNH). Meanwhile, the results in 10-cycle and solar-illuminated N 2 RR indicate the beveled CuAu nanoboxes are not only robust electrocatalysts but show promise in photocatalysis as well.

Metal-organic frameworks (MOFs) are significant useful molecular materials as a result of their high surface area and flexible catalytic activities by tuning the metal centers and ligands. MOFs have attracted great attention as efficient nanozymes recently; however, it is still difficult to understand polymetallic MOFs for enzymatic catalysis because of their complicated structure and interactions. Herein, bimetallic NiFe 2 MOF octahedra were well prepared and exhibited enhanced peroxidase-like activities. The synergistic effect of Fe and Ni atoms was systematically investigated by electrochemistry, X-ray photoelectron spectrometry, (XPS) and in situ Raman techniques. The electrons tend to transfer from Ni 2+ to Fe 3+ in NiFe 2 MOFs, and the resulting Fe 2+ is ready to decompose H 2 O 2 and generate · OH by a Fenton-like reaction. After integration with glucose oxidase (GOx), which can downgrade the pH value and generate H 2 O 2 by oxidation of glucose, a self-activated cascade reagent is therefore established for efficiently inducing cell death. The changes of cell morphology, DNA, and protein are also successfully recorded during the cell death process by Raman spectroscopy and fluorescence imaging.

Hydrogen is a fuel with a potentially zero-carbon footprint viewed as a viable alternative to fossil fuels. It can be produced in a large scale via electrochemical water splitting using electricity derived from renewable sources, but this would require highly active, inexpensive, and stable hydrogen evolution reaction (HER) catalysts to replace the Pt benchmark. Transition-metal phosphides (TMPs) are potential Pt replacements owing to their generally high activity as well as versatility as HER catalysts for different pH media. This review summarizes the recent progress in the development of TMP HER electrocatalysts, focusing on the strategies that have been recently explored to tune the activity in acidic, neutral, and basic media. These strategies are the doping of TMPs with metal and nonmetal elements, fabrication of multimetallic phosphide phases, and construction of multicomponent heterostructures comprising TMPs and another component such as a different TMP or a metal oxide/hydroxide. The synthetic methods utilized to design the catalysts are also presented. Finally, the challenges still remaining and future research directions are discussed.

Rapid, facile, and reliable recognition of different antibiotics by self-calibrating luminescent sensors are important for practical requirements. Herein, we design and synthesize a series of Eu 1- x Tb x -MOF using a flexible ligand H 4 L (5,5'-(propane-1,3-diylbis(oxy))di-isophthalic acid). With changing reactant time, submicrometer bimetallic SMOF-10-10h with homogeneous morphology was achieved and further fabricated MOF-based membrane combining with polymer materials. A luminescent study indicated that the bimetallic SMOF-10-10h membrane possesses a legible emission peak for Eu 3+ and Tb 3+ ions, which can act as a self-calibrating luminescent probe for efficiently sensing different antibiotics within a certain concentration range through two-dimensional (2D) readouts based on the emission intensity ratio. Our work first reports an inexpensive and convenience bimetallic MOF-based membrane as a luminescent sensor with self-calibrating to detect various antibiotics, which makes it a potential luminescent sensor for beneficial application.

Oxides are envisioned as promising catalysts to facilitate water oxidation, and the benign presence of hydroxide moieties can further enhance the catalyst performance. However, the nature of synergy between oxides and hydroxides remains elusive. In this study, we have designed a one-pot solution growth technique for the synthesis of flower-shaped N-doped-C-enveloped NiCo 2 O 4 /Ni x Co (1- x ) (OH) y catalysts with varying oxide and hydroxide contents and investigated their water oxidation behavior. The correlation between performance-determining parameters involved in water oxidation, such as the onset potential and overpotential with oxide and/or hydroxide content, oxidation states (oxides), and elemental composition (Co/Ni content), and the possible ways to achieve their optimal values are discussed in detail. Our observations conclude that the onset potential and overpotential are minimal for the hybrid oxide-hydroxide bimetallic system compared with pristine hydroxide or oxide. The optimal hybrid catalyst shows excellent current density, low Tafel slope (82 mV/dec), and low onset potential (281 mV at 2 mA/cm 2 ) and overpotential (348 mV at 10 mA/cm 2 ), besides enduring operational stability in alkaline medium. The low Tafel slope suggests the preferable kinetics for water oxidation, and the poisoning study reveals the direct involvement of metal as active sites. The overall study unveils the synergy in the Co-Ni-based binary transition-metal oxide-hydroxide hybrid, which makes it a potential candidate for water oxidation catalysts, and hence, it is expected that the hybrid will find applications in energy conversion devices, such as electrolyzers.

ZrO 2 nanotube arrays and their supported bimetallic platinum and ruthenium (Pt x Ru y /ZrO 2 ; x + y = 1 mmol %, x / y = 1:0, 0.9:0.1, 0.8:0.2, 0.7:0.3, 0.5:0.5, 0:1) nanocomposites were fabricated by employing SBA-15-OH as a hard template and an impregnation method, respectively. A controlled ordered nanotube array structure formed from the fabricated catalysts, and it showed a good performance for toluene oxidation. The specific physicochemical properties of the catalysts were examined through various analytical means. The Pt x Ru y /ZrO 2 possessed a high surface area, and the Pt-Ru nanoparticles were dispersed uniformly on the ZrO 2 nanotube surface. The Pt 0.7 Ru 0.3 /ZrO 2 catalyst performed best among all of the samples, with T 90% (temperatures for 90 and 100% conversion of toluene) of 140 and 160 °C, respectively, at a weight hourly space velocity of 36 000 mL/(h·g). These bimetallic catalysts exhibit excellent characteristics for toluene oxidation, such as higher turnover frequencies and lower apparent activation energy ( T 100% (temperatures for 90 and 100% conversion of toluene) of 140 and 160 °C, respectively, at a weight hourly space velocity of 36 000 mL/(h·g). These bimetallic catalysts exhibit excellent characteristics for toluene oxidation, such as higher turnover frequencies and lower apparent activation energy ( E a ) values, which probably result from the synergistic effect of the Pt-Ru noble metals that leads to a high reducibility and oxygen adsorption capacity. The excellent activity, stability, and economics of the Pt 0.7 Ru 0.3 /ZrO 2 catalyst allow for its application in toluene removal.

Bimetallic gold core-silver shell (Au@Ag) surface-enhanced Raman scattering (SERS) tags draw broad interest in the fields of biological and environmental analysis. In reported tags, silver coating tended to smooth the surface and merge the original hotspot of Au cores, which was disadvantageous to signal enhancement from the aspect of surface topography. Herein, we developed gold nanorod (AuNR)-bridged Au@Ag SERS tags with uniform three-dimensional (3D) topography for the first time. This unique structure was achieved by selecting waxberry-like Au nanoparticles (NPs) as cores, which were capped by vertically oriented AuNR arrays. Upon selective surface blocking with thiol-ligands, Ag NPs were controlled to anisotropically grow on the tips of the AuNRs, producing high-density homo- (Ag-Ag) and hetero- (Au-Ag) hotspots in a single NP. The 3D hotspots rendered this NP extraordinary SERS enhancement ability (an analytical enhancement factor of 3.4 × 10 6 ) 30 times higher than the counterpart with a smooth surface, realizing signal detection from a single NP. More importantly, multiplexing signals ("blank" or multiplex "internal standard") can be achieved by simply changing thiol-ligands, as exemplified in the synthesis of NPs with 8 signatures. Furthermore, the multifunctionality has been demonstrated in living cell/in vivo imaging, photothermal therapy, and SERS substrates for ratiometric quantitative analysis, relying on the inherent internal standard signal. The prepared Au@Ag NPs have great potential as standard tools in many SERS-related fields.

Understanding the microstructural evolution of bimetallic Pt nanoparticles under electrochemical polarization is critical to developing durable fuel cell catalysts. In this work, we develop a colloidal synthetic method to generate core-shell Au@Pt nanoparticles of varying surface Pt coverages to understand how as-synthesized bimetallic microstructure influences nanoparticle structural evolution during formic acid oxidation. By comparing the electrochemical and structural properties of our Au@Pt core-shells with bimetallic AuPt alloys at various stages in catalytic cycling, we determine that these two structures evolve in divergent ways. In core-shell nanoparticles, Au atoms from the core migrate outward onto the surface, generating transient "single-atom" Pt active sites with high formic acid oxidation activity. Metal migration continues until Pt is completely encapsulated by Au, and catalytic reactivity ceases. In contrast, AuPt alloys undergo surface dealloying and significant leaching of Pt out of the nanoparticle. Elucidating the dynamic restructuring processes responsible for high electrocatalytic reactivity in Pt bimetallic structures will enable better design and predictive synthesis of nanoparticle catalysts that are both active and stable.

Noble metals usually work as the cocatalyst for photocatalytic water splitting, but their rare and expensive properties narrowed their wide development. Transition-metal sulfides have appeared to be promising non-noble metal cocatalysts in the hydrogen evolution reaction (HER) to meet future energy demands. Meanwhile, many studies focus on the fabrication of bimetallic catalysts because of their remarkably superior catalytic activity compared with monometallic substances. Herein, amorphous bimetallic cobalt nickel sulfide (CoNiS x ) was fabricated to work as a cocatalyst in the photocatalytic H 2 evolution reaction, which can couple with pristine graphitic carbon nitride (g-C 3 N 4 ). CoNiS x -CN exhibits a larger specific surface area compared with g-C 3 N 4 , making it possess more reaction active sites. Moreover, the contacted interface in the CoNiS x -CN composite photocatalyst contributes to higher separation efficiency of photogenerated carriers, which was proved by experimental and theoretical calculations. More importantly, the theoretical calculation also verified that CoNiS x -CN has relatively closer Gibbs free energy to zero than pure g-C 3 N 4 and corresponding monometallic cocatalyzed g-C 3 N 4 . Therefore, the prepared CoNiS x -CN composite exhibited a dramatic photocatalytic HER performance of 2.366 μmol mg -1 h -1 , which is about 76-fold higher in comparison with pristine g-C 3 N 4 and comparable to g-C 3 N 4 with Pt as a cocatalyst under 420 nm light irradiation. This study reveals a promising and efficient bimetallic cocatalyst for the photocatalytic H 2 evolution reaction.

Herein, we report the synthesis of metal (Pt and Au) and metal alloy (PtAu) nanoparticles (NPs)-integrated graphitic carbon nitride (g-C 3 N 4 ) hybrids using a facile solvothermal route for water-splitting application. The metal and metal alloy NPs with varying percentages of Pt and Au are found to be in the size range of 3-5 nm and uniformly distributed on the g-C 3 N 4 sheets. The metal and metal alloy NPs act as cocatalyst for g-C 3 N 4 to enhance the photocatalytic activity for hydrogen (H 2 ) generation through higher light absorption and efficient charge separation. The alloy composition plays an important role to maximize the photoactivity, with an optimized PtAu/g-C 3 N 4 sample delivered 1009 μmol g -1 h -1 of H 2 . The visible light assisted photocatalytic H 2 evolution is further investigated with the optimized PtAu alloy NPs-integrated g-C 3 N 4 . This study presents a robust, stable, and easily synthesizable PtAu/g-C 3 N 4 hybrid material as a promising photocatalyst for H 2 generation through water splitting.

Hydrogen peroxide (H 2 O 2 ), a green oxidant, has wide applications in various chemical syntheses and is also a promising candidate to replace the traditional toxic oxidants. The direct synthesis of H 2 O 2 from H 2 and O 2 is a potential approach, as it is a green and atomically economic reaction. However, the most previous systems are notorious in complicated post-purification procedures, high energy cost, and low selectivity because of the uncontrollable O-O bond cleavage. We have solved this challenge by tuning the chemical state of Pd with high H 2 O 2 productivity of 80.4 mol kg cat -1 h -1 and high H 2 O 2 selectivity of 82.1% via the design of Pd-Ag nanoalloys with flexibly tuned size and composition. The created Pd-Ag nanoalloy also exhibits excellent stability with limited performance decay over recycles. The X-ray photoelectron spectroscopy analysis confirms the electron transfer from Ag to Pd, which generates more Pd 0 and enables improved H 2 O 2 productivity. The theoretical calculation shows that the incorporation of Ag into Pd is beneficial for the stabilization of O 2 2- and the cleavage of H 2 for the enhanced H 2 O 2 generation. In addition, the enhanced H 2 O 2 desorption on Pd-Ag nanoalloy is beneficial for releasing H 2 O 2 , which results in the increased H 2 O 2 selectivity.

Designing and exploring catalysts with high activity and stability for oxygen reduction reaction (ORR) at the cathode in acidic environments is imperative for the industrialization of proton exchange membrane fuel cells (PEMFCs). Theoretical calculations and experiments have demonstrated that alloying Pt with a transition metal can not only cut down the usage of scarce Pt metal but also improve performance of mass activity compared with pure Pt. Herein, we exhibit the preparation of nanoporous PtFe nanoparticles (np-PtFe NPs) supported on N-doped porous carbon sheets (NPCS) via facile in situ thermolysis of a Pt-modified Fe-based metal-organic framework (MOF). The np-PtFe/NPCS exhibit a more positive half-wave potential (0.92 V) compared with commercial Pt/C catalyst (0.883 V). The nanoporous structure allows our catalyst to possess high mass activity, which is found to be 0.533 A·mg Pt -1 and 3.04 times better than that of Pt/C (0.175 A·mg Pt -1 ). Moreover, the conversion of PtFe NPs from porous to hollow structure can maintain the activity of electrocatalyst. Our strategy provides a facile design and synthesis process of noble-transition metal alloy electrocatalysts via noble metal modified MOFs as precursors.

The development of inexpensive, efficient, and environmentally friendly catalysts for oxygen evolution reaction (OER) is of great significant for green energy utilization. Herein, binary metal oxides (M x Co 3-x O 4 , M = Zn, Ni, and Cu) with yolk-shell polyhedron (YSP) structure were fabricated by facile pyrolysis of bimetallic zeolitic imidazolate frameworks (MCo-ZIFs). Benefiting from the synergistic effects of metal ions and the unique yolk-shell structure, M x Co 3-x O 4 YSP displays good OER catalytic activity in alkaline media. Impressively, Zn x Co 3-x O 4 YSP shows a comparable overpotential of 337 mV at 10 mA cm -2 to commercial RuO 2 and exhibits superior long-term durability. The high activity and good stability reveals its promising application.

It can be difficult to simultaneously control the size, composition, and morphology of metal nanomaterials under benign aqueous conditions. For this, bioinspired approaches have become increasingly popular due to their ability to stabilize a wide array of metal catalysts under ambient conditions. In this regard, we used the R5 peptide as a three-dimensional template for formation of PdPt bimetallic nanomaterials. Monometallic Pd and Pt nanomaterials have been shown to be highly reactive toward a variety of catalytic processes, but by forming bimetallic species, increased catalytic activity may be realized. The optimal metal-to-metal ratio was determined by varying the Pd:Pt ratio to obtain the largest increase in catalytic activity. To better understand the morphology and the local atomic structure of the materials, the bimetallic PdPt nanomaterials were extensively studied by transmission electron microscopy, extended X-ray absorption fine structure spectroscopy, X-ray photoelectron spectroscopy, and pair distribution function analysis. The resulting PdPt materials were determined to form multicomponent nanostructures where the Pt component demonstrated varying degrees of oxidation based upon the Pd:Pt ratio. To test the catalytic reactivity of the materials, olefin hydrogenation was conducted, which indicated a slight catalytic enhancement for the multicomponent materials. These results suggest a strong correlation between the metal ratio and the stabilizing biotemplate in controlling the final materials morphology, composition, and the interactions between the two metal species.

Increased proliferation of antimicrobial resistance and new strains of bacterial pathogens severely impact current health, environmental, and technological developments, demanding design of novel, highly efficient antibacterial agents. Ag, Cu monometallic and Ag/Cu bimetallic nanoparticles (NPs) were in situ grown on the surface of graphene, which was produced by chemical vapor deposition using ferrocene as precursor and further functionalized to introduce oxygen-containing surface groups. The antibacterial performance of the resulting hybrids was evaluated against Escherichia coli cells and compared through a series of parametrization experiments of varying metal type and concentration. It was found that both Ag- and Cu-based monometallic graphene composites significantly suppress bacterial growth, yet the Ag-based ones exhibit higher activity compared to that of their Cu-based counterparts. Compared with well-dispersed colloidal Ag NPs of the same metal concentration, Ag- and Cu-based graphene hybrids display weaker antibacterial activity. However, the bimetallic Ag/CuNP-graphene hybrids exhibit superior performance compared to that of all other materials tested, i.e., both the monometallic graphene structures as well as the colloidal NPs, achieving complete bacterial growth inhibition at all metal concentrations tested. This striking performance is attributed to the synergistic action of the combination of the two different metals that coexist on the surface as well as the enhancing role of the graphene support.

Noble metal bimetallic nanomaterials have attracted a great deal of attention owing to the strong correlation between their morphology and chemical and physical properties. Even though the synthetic strategies for controlling the shapes of monometallic nanomaterials such as gold (Au) and silver (Ag) are well-developed, limited advances have been made with Au/Ag bimetallic nanomaterials to date. In this work, we demonstrate a highly complex in-plate and on-plate structural control of Au/Ag bimetallic nanoplates (Au/AgBNPLs) in contrast to conventional, simply structured, 1D and 2D, branched, and polyhedral nanomaterials. The polymer used in the synthesis of seeds plays a critical role in controlling the structure of the Au/AgBNPLs. The Au/AgBNPLs exhibit exceptionally high chemical stability against various chemical etchants and a versatile catalytic reactivity with biologically and environmentally relevant chemical species. Significantly, the reversible assembly formation of the Au/AgBNPLs is demonstrated by carrying out the surface-functionalization of the materials with thiol DNA, emphasizing the potential applications of the Au/AgBNPLs in various diagnostic and therapeutic purposes. Finally, the surface-enhanced Raman scattering (SERS) properties of the Au/AgBNPLs are experimentally and theoretically investigated, demonstrating a substantial potential of the Au/AgBNPLs as single-nanoparticle SERS probes. Electron microscopy, UV-vis spectroscopy, selected area electron diffraction (SAED), and energy-dispersive X-ray (EDX) spectroscopy are employed to analyze the structure and composition of the Au/AgBNPLs at the atomic level.

A synergistic bimetallic enzyme mimetic catalyst, three-dimensional (3D) graphene/Fe3O4-AuNPs, was successfully fabricated which exhibited flexibly switchable peroxidase-like activity. Compared to the traditional 2D graphene-based monometallic composite, the introduced 3D structure, which was induced by the addition of glutamic acid, and bimetallic anchoring approach dramatically improved the catalytic activity, as well as the catalysis velocity and its affinity for substrate. Herein, Fe3O4NPs acted as supporters for AuNPs, which contributed to enhance the efficiency of electron transfer. On the basis of the measurement of Mott-Schottky plots of graphene and metal anchored hybrids, the catalysis mechanism was elucidated by the decrease of Fermi level resulted from the chemical doping behavior. Notably, the catalytic activity was able to be regulated by the adsorption and desorption of single-stranded DNA molecules, which laid a basis for its utilization in the construction of single-stranded DNA-based colorimetric biosensors. This strategy not only simplified the operation process including labeling, modification, and imprinting, but also protected the intrinsic affinity between the target and biological probe. Accordingly, based on the peroxidase-like activity and its controllability, our prepared nanohybrids was successfully adopted in the visualized and label-free sensing detections of glucose, sequence-specific DNA, mismatched nucleotides, and oxytetracycline.

In this work, a simple but powerful method for controlling the size and surface morphology of AgAu nanodendrites is presented. Control of the number of Ag nanoparticle seeds is found to provide a fast and effective route by which to manipulate the size and morphology of nanoparticles produced via a combined galvanic replacement and reduction reaction. A lower number of Ag nanoparticle seeds leads to larger nanodendrites with the particles' outer diameter being tunable in the range of 45-148 nm. The size and surface morphology of the nanodendrites was found to directly affect their catalytic activity. Specifically, we report on the activity of these AgAu nanodendrites in catalyzing the gas-phase oxidation of benzene, toluene and o-xylene, which is an important reaction for the removal of these toxic compounds from fuels and for environmental remediation. All produced nanodendrite particles were found to be catalytically active, even at low temperatures and low metal loadings. Surprisingly, the largest nanodendrites provided the greatest percent conversion efficiencies.

Bimetallic magnetic iron-nickel (FeNi) nanocrystals (NCs) were synthesized through a one-pot synthetic wet chemistry method, and the morphology of the resulting NCs can be adjusted by changing the molar ratio of chemical attendees during the experimental processes. The obtained FeNi NCs can be redispersed in water medium though the phase works by using the ligand exchange procedures of cysteine (Cys), 5-aminovaleric acid (5AA), and glutathione (GSH), respectively. The synthesized NCs exhibited excellent magnetic properties with Hc (magnetic fields, ≈10(-3) T) and μa (initial permeability of up to 10(5)). Furthermore, linear sweep voltammetry (LSV) polarization curves revealed a low overpotential of -0.47, -0.44, and 0.15 V and a current of 105.7, 97.8, and 209 mA for the Cys-, 5AA-, and GSH-FeNi NCs, respectively. This indicated a relatively high catalytic activity of these NCs in the hydrogen evolution reaction (HER). The different cell lines (AGS, HepG2, MG63, NCI-H460, and SK-MEL-2) exposed to FeNi NCs for 5 days exhibited >87% viability at concentrations of up to 50 μg mL(-1), which was indicative of excellent biocompatibility. The resulting FeNi NCs offer a facile synthetic route to fabricate monodispersed NCs. The biocompatibility of these NCs should also enable their application in electrocatalysis and biological applications.

The design and development of well-defined, functional nanostructures via self-assembly is one of the key objectives in current nanotechnology. Block copolymer-based hybrid materials are attractive candidates for the fabrication of multifunctional nanostructures, which provide the building blocks for more complex nanoarchitectures and nanodevices. However, one of the major challenges lies in controlling the structure formation in these hybrid materials by guiding the self-assembly of the block copolymer. Here, hierarchical nanoporous structures are fabricated via guided multistep self-assembly of diblock copolymer micellar solutions onto hydrophilic solid substrates. The core of polystyrene-block-poly[4-vinylpyridine] micelles serves as a nanoreactor for the preparation of size-controlled gold nanoparticles. Deposition of thin films of the micellar solution in combination with a nonselective cosolvent (THF), on hydrophilic surfaces leads to the formation of hierarchical nanoporous structures. The micellar films exhibit two different pore diameters and a total pore density of more than 10(10) holes per cm2. Control over the pore diameter is achieved by adapting the molecular weight of the polystyrene-block-poly[4-vinylpyridine] diblock copolymer. Moreover, the porous morphology is used as a template for the fabrication of bimetallic nanostructured thin films. The PS-b-P4VP template is subsequently removed by oxygen plasma etching, leaving behind binary nanoparticle structures that mimic the original thin film morphology.

Developing robust antibacterial materials is of importance for a wide range of applications such as in biomedical engineering, environment, and water treatment. Herein we report the development of a novel superhydrophobic surface featured with hierarchical architecture and bimetallic composition that exhibits enhanced antibacterial activity. The surface is created using a facile galvanic replacement reaction followed by a simple thermal oxidation process. Interestingly, we show that the surface's superhydrophobic property naturally allows for a minimal bacterial adhesion in the dry environment, and also can be deactivated in the wet solution to enable the release of biocidal agents. In particular, we demonstrate that the higher solubility nature of the thermal oxides created in the thermal oxidation process, together with the synergistic cooperation of bimetallic composition and hierarchical architecture, allows for the release of metal ions in a sustained and accelerated manner, leading to enhanced antibacterial performance in the wet condition as well. We envision that the ease of fabrication, the versatile functionalities, and the robustness of our surface will make it appealing for broad applications.

Porous silica-coated hollow gold-silver nanoshells were successfully synthesized utilizing a procedure where the porous silica shell was produced prior to the transformation of the metallic core, providing enhanced control over the structure/composition of the bimetallic hollow core. By varying the reaction time and the precise amount of gold salt solution added to a porous silica-coated silver-core template solution, composite nanoparticles were tailored to reveal a readily tunable surface plasmon resonance that could be centered across the visible and near-IR spectral regions (∼445-800 nm). Characterization by X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy, scanning electron microscopy, and transmission electron microscopy revealed that the synthetic methodology afforded particles having uniform composition, size, and shape. The optical properties were evaluated by absorption/extinction spectroscopy. The stability of colloidal solutions of our composite nanoparticles as a function of pH was also investigated, revealing that the nanoshells remain intact over a wide range of conditions (i.e., pH 2-10). The facile tunability, enhanced stability, and relatively small diameter of these composite particles (∼110 nm) makes them promising candidates for use in tumor ablation or as photothermal drug-delivery agents.