Regulation of MRI contrast and cellular retention time by cellular interfacial distribution of Gd agents:Implications for stem cell tracking

Human mesenchymal stem cells(hMSCs)were labeled with Dotarem or(Gd-DOTA)2-EM7(EM7Gd2)via electroporation(EP).Cellular transmission electron microscopy(TEM)reveals free distribution of Gd agents and formation of EM7Gd2 clusters in the cytosol.Cellular magnetic resonance imaging(MRI)reveals that the free Gd agents induce MRI signal enhancement effect due to its fast exocytosis and subsequent interaction with intercellular water molecules.The EM7Gd2 clusters exhibits a longer intracellular retention time and induce a persistent MRI signal reduction effect.The cellular MRI results are interpreted by taking into account both T1 and T2 relaxation rates and their correlation with cellular binding structures of Dotarem and EM7Gd2.

Controllable Biosynthesis and Properties of Gold Nanoplates Using Yeast Extract

Biosynthesis of gold nanostructures has drawn increasing concerns because of its green and sustainable synthetic process. However, biosynthesis of gold nanoplates is still a challenge because of the expensive source and difficulties of controllable formation of morphology and size. Herein, one-pot biosynthesis of gold nanoplates is proposed, in which cheap yeast was extracted as a green precursor. The morphologies and sizes of the gold nanostructures can be controlled via varying the pH value of the biomedium. In acid condition, gold nanoplates with side length from 1300 ± 200 to 300 ± 100 nm and height from 18 to 15 nm were obtained by increasing the pH value. Whereas, in neutral or basic condition, only gold nanoflowers and nanoparticles were obtained. It was determined that organic molecules, such as succinic acid, lactic acid, malic acid, and glutathione, which are generated in metabolism process, played important role in the reduction of gold ions. Besides, it was found that the gold nanoplates exhibited plasmonic property with prominent dipole infrared resonance in near-infrared region, indicating their potential in surface plasmon-enhanced applications, such as bioimaging and photothermal therapy.

In situ construction of thiol-silver interface for selectively electrocatalytic CO_(2)reduction

Electrochemical CO_(2)reduction(ECR)is one of the most effective methods to obtain carbonaceous chemicals and reduce greenhouse gases passingly under the ambient condition.However,efficient electrocatalysts featured with high selectivity and stability are still lacking.A novel molecule-mediated Ag electrocatalyst with capped thiols is rationally designed for high-performance ECR.The thiol-capped and carbon-supported Ag nanostructures(Ag-TC)are formed by in situ electrochemical reduction from three-dimentional(3D)Ag-thiol metal-organic compound with cysteine as the anchor agent and carbon source.Ag-TC exhibits high selectivity and stability for CO_(2)conversion to CO(86.7%),which is more catalytically active than that of common Ag nanoparticles.The function of thiols for ECR is proved by replacing cysteine with alanine without thiol group.Meanwhile,alternatively replacing and removing the surface molecules on the Ag foil further demonstrate the effct of thiols.This work enlightens the promise of in situ construction method for molecule capped metal electrocatalyst towards selective and stable ECR.

Erratum to:In situ construction of thiol-silver interface for selectively electrocatalytic CO_(2)reduction

Erratum to Nano Research 2022,15(4):3283−3289 https://doi.org/10.1007/s12274-021-3978-7 One funding number in the Acknowledgements section was unfortunately mistakenly used.This error did not affect any of the conclusions from the published paper.

超亲水纳孔分离膜的制备及其分子分离性能和稳定性研究

膜分离技术在有机分子污水的处理中具有广泛应用,其面临的难题之一是制备具有超亲水性质的纳孔膜以抵御有机污染物的污染,实现高效、稳定的分子分离.在本文中,我们通过全膜交联的方法在保持水凝胶纳孔膜超亲水性质的前提下大幅提升了其机械强度,制备了高强度超亲水纳孔膜.该膜实现了有机分子的高效分离,水通量达到220 L m^(-2)h^(-1)bar^(-1),考马斯亮蓝(CBB)截留率达到~99.9%,分子/盐(CBB/Na_(2)SO_(4))选择性达到747.在以腐殖酸为污染物的分子分离中,该膜表现出优异的抗污染性能,通量恢复率接近100%.该膜还具有出色的抗压性能,在高达8 bar的跨膜压力下保持了稳定的分子分离性能.本工作为制备超亲水纳孔膜实现有机分子废水的高效分离提供了一种新的思路.

An intelligent DNA nanodevice for precision thrombus therapy

Obstruction of blood vessels(thrombosis)due to blood clots is one of the main causes of death worldwide and is associated with many cardiovascular diseases,such as myocardial infarction,ischemic stroke,and pulmonary embolism[1].Thrombolytic therapy is currently the preferred treatment for acute thrombosis and is administered intravenously with thrombolytic drugs,such as tissue plasminogen activator(tPA)[2].

Flexible bidirectional self-powered photodetector with significantly reduced volume and accelerated response speed based on hydrogel and lift-off GaN-based nanowires

Due to the wide range of potential applications for next-generation multi-functional devices,the flexible selfpowered photodetector(PD)with polarity-switchable behavior is essential but very challenging to be realized.Herein,a wearable bidirectional self-powered PD based on detached(Al,Ga)N and(In,Ga)N nanowires has been proposed and demonstrated successfully.Arising from the photovoltage-competing dynamics across(Al,Ga)N and(In,Ga)N nanowire photoelectrodes,such PD can generate the positive(33.3 mA W−1)and negative(-0.019 mA W−1)photo-responsivity under ultraviolet(UV)and visible illumination,respectively,leading to the bidirectional photocurrent behavior.Thanks to the introduction of quasi solid-state hydrogel,the PD can work without the liquid-electrolyte,thus remarkably reducing the volume from about 482 cm3 to only 0.18 cm3.Furthermore,the use of hydrogel is found to enhance response speed in the UV range by reducing the response time for more than 95%,which is mainly attributed to the increased open circuit potential and reduced ion transport distance.As the GaN connecting segment is pretty thin,the piezoelectric charges generated by stress are proposed to have only a limited effect on the photocurrent density.Therefore,both the stable on-off switching characteristics and photocurrent densities can still be achieved after being bent 400 times.With an excellent flexibility,this work creates opportunities for technological applications of bidirectional photocurrent PDs in flexible optoelectronic devices,e.g.,wearable intelligent sensors.

Thiol-Disulfide Exchange Coordinates the Release of Nitric Oxide and Dexamethasone for Synergistic Regulation of Intestinal Microenvironment in Colitis

The cell-specific functions of nitric oxide(NO)in the intestinal microenvironment orchestrate its therapeutic effects in ulcerative colitis.While most biomaterials show promise by eliciting the characteristics of NO,the insufficient storage,burst release,and pro-inflammatory side effects of NO remain as challenges.Herein,we report the development of thiol-disulfide hybrid mesoporous organosilica nanoparticles(MONs)that improve the storage and sustained release of NO,broadening the therapeutic window of NO-based therapy against colitis.The tailored NO-storing nanomaterials coordinated the release of NO and the immunoregulator dexamethasone(Dex)in the intestinal microenvironment,specifically integrating the alleviation of oxidative stress in enterocytes and the reversal of NO-exacerbated macrophage activation.Mechanistically,such a synchronous operation was achieved by a self-motivated process wherein the thiyl radicals produced by NO release cleaved the disulfide bonds to degrade the matrix and release Dex via thiol-disulfide exchange.Specifically,the MON-mediated combination of NO and Dex greatly ameliorated intractable colitis compared with 5-aminosalicylic acid,even after delayed treatment.Together,our results reveal a key contribution of synergistic modulation of the intestinal microenvironment in NO-based colitis therapy and introduce thiol-disulfide hybrid nanotherapeutics for the management of inflammatory diseases and cancer.

Manipulating exciton confinement for stable and efficient flexible quantum dot light-emitting diodes

Flexible quantum dot light-emitting diodes(QLEDs)show great promise for the next generation of flexible,wearable,and artificial intelligence display applications.However,the performance of flexible QLEDs still lags behind that of rigid substrate devices,hindering their commercialization for display applications.Here we report the superior performance of flexible QLEDs based on efficient red ZnCdSe/ZnS/ZnSe QDs(A-QDs)with antitype-I nanostructures.We reveal that using ZnS as an intermediate shell can effectively confine the exciton wavefunction to the inner core,reducing the surface sensitivity of the QDs and maintaining its excellent emission properties.These flexible QLEDs exhibit a peak external quantum efficiency of 23.0%and a long lifetime of 63,050 h,respectively.The anti-type-I nanostructure of A-QDs in the device simultaneously suppresses defectinduced nonradiative recombination and balances carrier injection,achieving the most excellent performance of flexible QLEDs ever reported.This study provides new insights into achieving superior performance in flexible QD-based electroluminescent devices.

Advanced near-infrared light approaches for neuroimaging and neuromodulation

Almost all physiological processes of animals are controlled by the brain,including language,cognitive,memory,learning,emotion and so forth.Minor brain dysfunction usually leads to brain diseases and disorders.Therefore,it'is greatly meaningful and urgent for scientists to have a better understanding of brain structure and function.Optical approaches can provide powerful tools for imaging and modulating physiological processes of the brain.In particular,optical approaches in the near-infrared(NIR)window(700-1700 nm)exhibit excellent prosperities of deep tissue penetration and low tissue scattering and absorption compared with those of visible windows(400-700 nm),which provides a promising approach for scientists to develop desired methods of neuroimaging and neuromodulation in deep brain tissues.In this review,variable types of NIR light approaches for imaging and modulating neural ions,membrane potential,neurotransmitters,and other critical molecules for brain functions and diseases are summarized.In particular,the latest breakthrough research of brain imaging and brain regulation in the NIR-II window(1000-1700 nm)are highlighted.Finally,we conclude the challenges and prospects of NIR light-based neuroimaging and neuromodulation for both basic brain research and further clinical translation.

The activity of Zn precursors determines the cation exchange reaction kinetics with Ag_(2)S:Zn-doped Ag_(2)S or Ag_(2)S@ZnS QDs

Cation exchange(CE)has been emerged as a promising post-synthesis strategy of colloidal nanocrystals.However,it is unclear how the cation precursor affects the CE process and the final colloidal nanocrystals.Herein,we utilized two Zn-B Lewis acidbase adduct complexes(B=oleylamine(OAM)and methanol(MeOH))as Zn precursors for CE with Ag_(2)S quantum dots(QDs).Our study revealed that the steric hindrance and complexing capabilities of Zn precursor significantly affect the CE kinetics.As a result,the Zn-doped Ag_(2)S(Zn:Ag_(2)S)and Ag_(2)S@ZnS core–shell QDs were successfully obtained with enormous enhancement of their photoluminescence(PL)intensities.Theoretical simulation showed that the Zn-OAM with higher desolvation energy and spatial hindrance tended to form doped Zn:Ag_(2)S QDs due to the inefficient cation exchange.Whereas the Zn-MeOH with lower exchange barrier promoted the conversion of Ag-S to Zn-S,thus forming Ag_(2)S@ZnS core–shell QDs.We anticipate that this finding will enrich the regulatory approaches of post-synthesis of colloidal nanocrystals with desirable properties.

Controlled synthesis of porous spinel cobalt manganese oxides as efficient oxygen reduction reaction electrocatalysts

In this article, we report a facile precursor pyrolysis method to prepare porous spinel-type cobalt manganese oxides （CoxMng-xO4） with controllable morphologies and crystalline structures. The capping agent in the reaction was found to be crucial on the formation of the porous spinel cobalt manganese oxides from cubic Co2MnO4 nanorods to tetragonal CoMn2O4 microspheres and tetragonal CoMn204 cubes, respectively. All of the prepared spinel materials exhibit brilliant oxygen reduction reaction （ORR） electrocatalysis along with high stability. In particular, the cubic Co2MnO4 nanorods show the best performance with an onset potential of 0.9 V and a half-wave potential of 0.72 V which are very close to the commercial Pt/C. Meanwhile, the cubic Co2MnO4 nanorods present superior stability with negligible degradation of their electrocatalytic activity after a continuous operation time of 10,000 seconds, which is much better than the commercial Pt/C electrocatalvst.

MoSe2 porous microspheres comprising monolayer flakes with high electrocatalytic activity

A facile colloidal route to synthesize MoSe2 porous microspheres with diameters of 400-600 nm made up of MoSe2 monolayer flakes （-0.7 nm in thickness） is reported. The solvents trioctylamine （TOA） and oleylamine （OAM） are found to play important roles in the formation of MoSe2 microspheres, whereby TOA determines the three-dimensional （3D） microspherical morphology and OAM directs the formation of MoSes monolayer flakes. The robust 3D MoSe2 microspheres exhibit remarkable activity and durability for the electrocatalytic hydrogen evolution reaction （HER） in acid, maintaining a small onset overpotential of -77 mV and keeping a small overpotential of 100 mV for a current density of 5 mA/cm2 after 1,000 cycles. In addition, similar 3D WSe2 microspheres can also be prepared by using this method. We expect this facile colloidal route could further be expanded to synthesize other porous structures which will find applications in fields such as in energy storage, catalysis, and sensing.

Facile synthesis of magnetic-plasmonic nanocomposites as T1 MRI contrast enhancing and photothermal therapeutic agents

Nanocomposites combining magnetic and plasmonic components have received widespread attention in recent years due to their potential applications in biomedical research. Herein, we describe a facile method for growing small iron oxide nanoparticles on various plasmonic core materials with different shapes and surfaces by utilizing a polypyrrole interlayer. By focusing on Au nanorod@polypyrrole@iron oxide （Au NR@PPy@FexO） nanocomposites, we show that these systems exhibit a low r2/rl ratio of 4.8, making them efficient T1 positive contrast-enhancing agents for magnetic resonance imaging （MRI）. Moreover, we show that the nanocomposites are excellent photothermal agents in the second near infrared region, with high photothermal conversion efficiency, reaching up to 46%. In addition, the Au NR@PPy@FexO nanocomposites show very low cytotoxicity. In summary, the present results highlight the great potential of the synthetic method and the nanocomposites developed in this study for T~ MRI and/or infrared thermal imaging-guided photothermal cancer therapeutic applications.

Real-time in vivo visualization of tumor therapy by a near-infrared-II Ag2S quantum dot-based theranostic nanoplatform

Real-time and objective feedback of therapeutic efficacies would be of great value for tumor treatment. Here, we report a smart Ag2S QD-based theranostic nanoplatform （DOX@PEG-Ag2S） obtained by loading the anti-cancer drug doxorubicin （DOX） into polyethylene glycol-coated silver sulfide quantum dots （PEG-Ag2S QDs） through hydrophobic-hydrophobic interactions, which exhibited high drug loading capability （93 wt.% of DOX to Ag2S QDs）, long circulation in blood （t1/2 = 10.3 h）, and high passive tumor-targeting efficiency （8.9% ID/gram） in living mice where % ID/gram reflects the probe concentration in terms of the percentage of the injected dose （ID） per gram of tissue. After targeting the tumor tissue, DOX from PEG-AgRS cargoes was selectively and rapidly released into cancer cells, giving rise to a significant tumor inhibition. Owing to the deep tissue penetration and high spatio-temporal resolution of Ag2S QDs fluorescence in the second near-infrared window （NIR-II）, the DOX@PEG-Ag2S enabled real-time in vivo reading of the drug targeting process and therapeutic efficacy. We expect that such a novel theranostic nanoplatform, DOX@PEG-Ag2S, with integrated drug delivery, therapy and assessment functionalities, will be highly useful for personalized treatments of tumors.

1.82 wt.% Pt/N, P co-doped carbon overwhelms 20 wt.% Pt/C as a high-efficiency electrocatalyst for hydrogen evolution reaction

Cost-effective electrocatalysts for the hydrogen evolution reaction （HER） play a key role in the field of renewable energy. Although tremendous efforts have been devoted to the search of alternative materials, Pt/C is still the most efficient electrocatalyst for the HER. Nevertheless, decreasing the loading of Pt in the designed eletrocatalysts is of significance. However, with low Pt loading, it is challenging to maintain excellent catalytic performance. Herein, a new catalyst （Pt/NPC） was prepared by dispersing Pt nanoparticles （PtNPs） with an average diameter of 1.8 nm over a three-dimensional （3D） carbon network co-doped with N and P. Because of the high electronegativity of the N and P dopants, PtNPs were uniformly dispersed on the carbon network via high electronic affinity between Pt and carbon, affording a Pt/NPC catalyst; Pt/NPC exhibited superior HER activity, attributed to the down-shift of the Pt d-band caused by the donation of charge from N and P to Pt. The results show that Pt/NPC with an ultralow Pt loading of 1.82 wt.% exhibits excellent HER performance, which corresponds to a HER mass activity 20.6-fold greater than that observed for commercial 20% Pt/C at an overpotential of 20 mV vs. RHE.

Bioinspired membranes for multi-phase liquid and molecule separation

Water pollution is a serious problem around the world. It causes the lack of clean drinking water and brings risks to human health.Membrane technology has become a competitive candidate to treat the contaminated wastewater due to its high separation efficiency and low energy consumption. In this review, we introduce the recent development of several kinds of bioinspired separation membranes, involving the membrane design and applications. We emphasize the multi-phase liquid separation membranes inspired from nature with special wettability applied for oil/water separation, organic liquids mixture separation, and emulsion separation. After separating multi-phase liquids using these membranes, small molecule pollutants still exist in singlephase liquid. Therefore, we also expand the scope to small molecule-scale separation membranes, such as the nacre-like graphene oxide separation membrane and other nanofiltration membranes. Summary and outlook concerning the future development of separation membranes are also introduced briefly.

Green synthesis of NiFe LDH/Ni foam at room temperature for highly efficient electrocatalytic oxygen evolution reaction

Clean energy technologies such as water splitting and fuel cells have been intensively pursued in the last decade for their free pollution. However, there is plenty of fossil energy consumed in the preparation of the catalysts,which results in a heavy pollution. Therefore, it is much desired but challenging to fabricate high-efficiency catalysts without extra energy input. Herein, we used a facile one-pot room-temperature method to synthesize a highly efficient electrocatalyst of nickel iron layered double hydroxide grown on Ni foam(NiFe LDH/NF) for oxygen evolution reaction(OER). The formation of the NiFe LDH follows a dissolutionprecipitation process, in which the acid conditions by hydrolysis of Fe^3+ combined with NO3^- could etch the NF to form Ni^2+. Then, the obtained Ni^2+ was co-precipitated with the hydrolysed Fe^3+ to in situ generate NiFe LDH on the NF. The NiFe LDH/NF exhibits excellent OER performance with a low potential of about 1.411 V vs. reversible hydrogen electrode(RHE) at a current density of 10 m A cm^-2, a small Tafel slope of 42.3 mV dec^-1 and a significantly low potential of ~1.452 V vs. RHE at 100 mA cm^-2 in 1 mol L^-1 KOH. Moreover, the material also keeps its original morphology and structure over 20 h. This energy-efficient strategy to synthesize NiFe LDH is highly promising for widespread application in OER catalyst industry.

Atomic-scale Pt clusters decorated on porousα-Ni(OH)_2 nanowires as highly efficient electrocatalyst for hydrogen evolution reaction

The synthesis of atomic-scale metal catalysts is a promising but very challenging project. In this work, we successfully fabricated a hybrid catalyst of PL/Ni（OH）2 with atomic-scale Pt clusters uniformly decorated on porous Ni（OH）2 nanowires （NWs） via a facile room-temperature synthesis strategy. The as-obtained Ptc/Ni（OH）2 catalyst exhibits highly efficient hydrogen evolution reaction （HER） performance under basic conditions. In 0.1moll-1 KOH, the Ptc/Ni（OH）2 has an onset overpotential of -0 mV vs. RHE, and a significantly low overpotential of 32 mV at a current density of 10mAcm-2, lower than that of the com- mercial 20% Pt/C （58 mV）. The mass current density data illustrated that the PL/Ni（OH）2 reached a high current den- sity of 6.34Amg^-1i at an overpotential of 50 mV, which was approximately 28 times higher than that of the commercial Pt/C （0.223Amg^-1i） at the same overpotential, proving the high-efficiency electrocatalytic activity of the as-obtained Ptc/Ni（OH）2 for HER under alkaline conditions.

Development and analysis of a novel AF11-2 aptamer capable of enhancing the fluorescence of aflatoxin B1

Aflatoxin B1(AFB1)is one of the most common mycotoxins that threatens human health.As singlestranded oligonucleotides with high affinity and specificity,aptamers have incomparable effect on the targeted detection of AFB1.Herein,after 11 rounds of selection and analysis using a modified affinity chromatography-based SELEX strategy,the truncated 37 nt aptamer AF11-2 was successfully obtained.The aptamer shows good detection performance for AFB1,and can sensitively detect AFB1 in the range of 100-1000 nmol/L,with a detection limit of 42 nmol/L.In the detection of pretreated edible peanut oil samples,AF11-2 aptamer also showed a high recovery rate and good stability for AFB1,and achieved satisfactory results.In addition,AF11-2 aptamer can significantly enhance the fluorescence ability of AFB1,which is not available in traditional Afla17-2-3 aptamer.After molecular docking analysis,it was found that AF11-2 and Afla17-2-3 had different nucleotide binding sites for AFB1.Afla17-2-3 binds to the carbonyl O of AFB1,while AF11-2 binds to the pyrrolic O of AFB1,which may be the main reason that AF11-2 can enhance the fluorescence of AFB1.