Early and precise cancer diagnosis substantially improves patient survival. Recent work has revealed that the levels of multiple microRNAs in serum are informative as biomarkers for the diagnosis of ...cancers. Here, we designed a DNA molecular computation platform for the analysis of miRNA profiles in clinical serum samples. A computational classifier is first trained in silico using miRNA profiles from The Cancer Genome Atlas. This is followed by a computationally powerful but simple molecular implementation scheme using DNA, as well as an effective in situ amplification and transformation method for miRNA enrichment in serum without perturbing the original variety and quantity information. We successfully achieved rapid and accurate cancer diagnosis using clinical serum samples from 22 healthy people (8) and people with lung cancer (14) with an accuracy of 86.4%. We envision that this DNA computational platform will inspire more clinical applications towards inexpensive, non-invasive and rapid disease screening, classification and progress monitoring.
Artificial nanorobots that can recognize molecular triggers and respond with programable operations provide an inspiring proof‐of‐principle for personalized theragnostic applications. We have ...constructed an intelligent DNA nanorobot for autonomous blood anticoagulation in human plasma. The DNA nanorobot comprises a barrel‐shaped DNA nanostructure as the framework and molecular reaction cascades embedded as the computing core. This nanorobot can intelligently sense the concentration of thrombin in the local environment and trigger an autonomous anticoagulation when excess thrombin is present. The triggering concentration of thrombin at which the nanorobot responds can be tuned arbitrarily to avoid possible side effects induced by excess thrombin. This makes the nanorobot useful for autonomous anticoagulation in various medical scenarios and inspires a more efficient and safer strategy for future personalized medicine.
A DNA nanorobot is presented that can intelligently regulate thrombin functions when it senses an over‐boosted coagulation environment. Under normal coagulation conditions it does not perform. The trigger concentrations of nanorobot can be tuned arbitrarily, which makes the nanorobot useful for autonomous anticoagulation in various medical scenarios and inspires a more efficient and safer strategy for personalized medicine.
Analyzing complex single‐nucleotide‐polymorphism (SNP) combinations in the genome is important for research and clinical applications, given that different SNP combinations can generate different ...phenotypic consequences. Recent works have shown that DNA‐based molecular computing is powerful for simultaneously sensing and analyzing complex molecular information. Here, we designed a switching circuit‐based DNA computational scheme that can integrate the sensing of multiple SNPs and simultaneously perform logical analysis of the detected SNP information to directly report clinical outcomes. As a demonstration, we successfully achieved automatic and accurate identification of 21 different blood group genotypes from 83 clinical blood samples with 100 % accuracy compared to sequencing data in a more rapid manner (3 hours). Our method enables a new mode of automatic and logical sensing and analyzing subtle molecular information for clinical diagnosis, as well as guiding personalized medication.
A general DNA computational strategy for automatically correlating detected single nucleotide mutation (including insertions, deletions and SNPs) based information to phenotypic outcomes by integration of multiplexed sensing and logical analysis is reported.
The effect of the molecular orientation distribution of the first monolayer of donor molecules at the hole-harvesting contact in an organic photovoltaic (OPV) on device efficiency was investigated. ...Two zinc phthalocyanine (ZnPc) phosphonic acids (PA) deposited on indium tin oxide (ITO) electrodes are compared: ZnPc(PA)4 contains PA linkers in all four quadrants, and ZnPcPA contains a PA linker in one quadrant. ZnPcPA monolayers exhibited a broad distribution of molecular orientations whereas ZnPc(PA)4 adsorption produced a monolayer with a narrower orientation distribution with the molecular plane more parallel to the ITO surface. We used potential-modulated attenuated total reflectance spectroelectrochemistry (PM-ATR) to characterize the charge-transfer kinetics of these films and show that the highest rate constants correspond to ZnPc subpopulations that are oriented more parallel to the ITO surface plane. For ZnPc(PA)4, rate constants exceeded 104 s–1 and are among the highest ever reported for a surface-confined redox couple, which is attributable to both its orientation and the small ZnPc–electrode separation distance. The performance of OPVs with ITO hole-harvesting contacts modified with ZnPc(PA)4 was comparable to that achieved with highly activated bare ITO contacts, whereas for ZnPcPA-modified contacts, the OPV performance was similar to that observed with (hole-blocking) alkyl-PA modifiers. These results demonstrate the synergism between molecular structure, energetics, and dynamics at interfaces in OPVs.
Artificial nanorobots that can recognize molecular triggers and respond with programable operations provide an inspiring proof‐of‐principle for personalized theragnostic applications. We have ...constructed an intelligent DNA nanorobot for autonomous blood anticoagulation in human plasma. The DNA nanorobot comprises a barrel‐shaped DNA nanostructure as the framework and molecular reaction cascades embedded as the computing core. This nanorobot can intelligently sense the concentration of thrombin in the local environment and trigger an autonomous anticoagulation when excess thrombin is present. The triggering concentration of thrombin at which the nanorobot responds can be tuned arbitrarily to avoid possible side effects induced by excess thrombin. This makes the nanorobot useful for autonomous anticoagulation in various medical scenarios and inspires a more efficient and safer strategy for future personalized medicine.
A DNA nanorobot is presented that can intelligently regulate thrombin functions when it senses an over‐boosted coagulation environment. Under normal coagulation conditions it does not perform. The trigger concentrations of nanorobot can be tuned arbitrarily, which makes the nanorobot useful for autonomous anticoagulation in various medical scenarios and inspires a more efficient and safer strategy for personalized medicine.
Using a monolayer of zinc phthalocyanine (ZnPcPA) tethered to indium tin oxide (ITO) as a model for the donor/transparent conducting oxide (TCO) interface in organic photovoltaics (OPVs), we ...demonstrate the relationship between molecular orientation and charge-transfer rates using spectroscopic, electrochemical, and spectroelectrochemical methods. Both monomeric and aggregated forms of the phthalocyanine (Pc) are observed in ZnPcPA monolayers. Potential-modulated attenuated total reflectance (PM-ATR) measurements show that the monomeric subpopulation undergoes oxidation/reduction with k s,app = 2 × 102 s–1, independent of Pc orientation. For the aggregated ZnPcPA, faster orientation-dependent charge-transfer rates are observed. For in-plane-oriented Pc aggregates, k s,app = 2 × 103 s–1, whereas for upright Pc aggregates, k s,app = 7 × 102 s–1. The rates for the aggregates are comparable to those required for redox-active interlayer films at the hole-collection contact in organic solar cells.
Thermoresponsive poly(N-isopropylacrylamide) (PNiPAAm) was covalently tethered to nanosilicate platelets (NSP) to generate a new class of organic−inorganic hybrid that exhibits self-assembly and ...phase transformation properties under applied stimuli. Hybrids of two grafting densities were prepared and the PNiPAAm length was precisely controlled to yield a degree of polymerization of 350−1890 and a narrow molecular weight distribution (1.21−1.50 polydispersity or M w/M n). Two distinctive second-order transitions were observed during differential scanning calorimetry analysis, indicating the existence of dual-segment density zones. The difference between the two transition temperatures gradually vanished with increasing chain length, and a single endothermic first-order transition emerged. The hybrid also underwent a heat-induced phase transformation after treatment with several heating and cooling cycles. It is believed that fixation of PNiPAAm onto NSP greatly inhibited chain relaxation movements and hindered reversible coil−globule transitions. Furthermore, thermally induced self-assembly behavior was directly observed by transmission electronic microscopy of the hybrid coating as a thin film on a silicon wafer surface. The formation of a 3D network of nanostructures was directed by the platelet shape at temperatures higher than the critical solution temperature of the PNiPAAm chains. The temperature-controllable phase separation for formation of an ordered domain network of 100−500 nm in dimension has potential for the fabrication of new smart nanomaterials.
Thermo-responsive nanoarrays with LCST: 32°C of AgNP/NSP-PNiPAAm nanosheets interact with different surface energy bacteria, such as hydrophilic B. subtilis and hydrophobic E. coli, at lower than ...LCST: 28°C and higher than LCST: 37°C for antibacterial applications.
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•Thermal-sensitive nanohybrids were fabricated for antibacterial applications.•The surface energy of nanohybrids with the selective adhesion of different bacteria was modulated at lower and higher than LCST: 32 oC.•The key point of antibacterial ability is the aggregation of Ag nanoparticles by PNiPAAm shrinkage at 37°C.
The ternary nanohybrids of silver nanoparticles (AgNPs) in combination with silicate nanoplatelets (NSP) and thermally sensitive poly(N-isopropylacrylamide) (PNiPAAm) were fabricated for antibacterial applications. PNiPAAm were chemically grafted on the NSP by atom-transfer radical polymerization (ATRP) via polymerizing N-isopropylacrylamide monomers with sol-gel linkers (BBTES). The nanoparticles of AgNPs then were adsorbed on NSP-PNiPAAm nanosheets through in situ reduction reaction of AgNO3 in aqueous dispersion. The particle sizes of AgNPs were estimated to be 7–12nm in diameter with different composition ratios of AgNPs to NSP-PNiPAAm, evaluated by transmission electron microscope (TEM). The nanohybrids of AgNP/NSP-PNiPAAm exhibited the unique property of lowest critical solution temperature (LCST) at 32°C. The thermo-responsive antibacterial efficacy of the ternary nanohybrids was demonstrated by Bacillus subtilis (B. subtilis) and Escherichia coli (E. coli) at lower than the LCST (28°C) and higher than the LCST (37°C). The result show that the great antibacterial ability was observed in the hydrophilic bacteria (B. subtilis) at 28°C. In contrast, the excellent antibacterial ability was found in the hydrophobic bacteria (E. coli) at 37°C, due to the surface energy modulation of AgNP/NSP-PNiPAAm. The tailoring of silver-containing ternary nanohybrids allow the new antibacterial nanomaterials to selectively affect the surface of bacteria by varying temperature.
The nano silicate platelets (NSPs) of 100 × 100 × 1 nm3 in dimension were previously derived from the exfoliation of naturally occurring sodium montmorillonite clay, and their affinity to the surface ...of bacteria was revealed. The unique characteristics of ionic charges (Si–O–Na+) and the presence of siloxanol functionalities (Si–OH) allowed the organic modification of NSP to form NSP-tethering poly(hydroxyethyl methacrylate) (PHEMA) pendants through a sol–gel and living polymerization. By attaching nathphalimide-type fluorescence onto NSP-PHEMA, a new class of fluorescent organic–inorganic hybrid (NSP-PHEMA-HA), was prepared and its photoluminescence (PL) and bacterial trapping properties were characterized. The investigation of PL emission revealed that the fluorescent NSP hybrids could be used to detect bacteria and possess the potential for the biosensor applications.
Analyzing complex single‐nucleotide‐polymorphism (SNP) combinations in the genome is important for research and clinical applications, given that different SNP combinations can generate different ...phenotypic consequences. Recent works have shown that DNA‐based molecular computing is powerful for simultaneously sensing and analyzing complex molecular information. Here, we designed a switching circuit‐based DNA computational scheme that can integrate the sensing of multiple SNPs and simultaneously perform logical analysis of the detected SNP information to directly report clinical outcomes. As a demonstration, we successfully achieved automatic and accurate identification of 21 different blood group genotypes from 83 clinical blood samples with 100 % accuracy compared to sequencing data in a more rapid manner (3 hours). Our method enables a new mode of automatic and logical sensing and analyzing subtle molecular information for clinical diagnosis, as well as guiding personalized medication.
A general DNA computational strategy for automatically correlating detected single nucleotide mutation (including insertions, deletions and SNPs) based information to phenotypic outcomes by integration of multiplexed sensing and logical analysis is reported.
