BULLETIN OF THE KOREAN CHEMICAL SOCIETY
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2017
·Vol. 38
·期 10
·1143-1148
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IF 0.602
Mingjing Zou,Shuyu Wang
We report a visualization assay for carcinoembryonic antigen (CEA). The assay was prepared based on target-specific recognition, aptamer-based DNAzyme self-catalysis, and colorimetric reaction. Aptamer of CEA was gathered at the surface of magnetic beads for sandwiched co-conjugate when CEA was added. The second aptamer (Apt2) on the beads was folded into G-quadruplex by KCl to make G-quadruplex-hemin DNAzyme with hemin. Apt2-based DNAzyme catalyzed H 2 O 2 -mediated oxidation of 3,3′,5,5′-tetramethylbenzidine, resulting in color changes and significant increase in absorption intensity at 450 nm (Δ A 450nm ). Yellow products can be observed with naked eyes when over 1.0 ng/mL CEA was added and there was a linear correlation between Δ A 450 nm and CEA concentrations in the range of 0.1–8.0 ng/mL with the detection limit of 0.06 ng/mL. The proposed method was then used to determine CEA in human serum from healthy people and tumor patients, revealing a correlation with data from the electrochemiluminescent immunoassay. Owing to its simplicity, selectivity, and low-cost, this method is a promising candidate for detecting CEA and clinical diagnosis of cancer.
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TALANTA
·
2017
·
IF 4.162
Mingmin Wu,Xiaoyong Wang,Kun Wang,Zijian Guo
Trypsin and its inhibitors are relevant to many physiological processes and diseases. In this study, a nanosensor capable of detecting trypsin and its inhibitors was designed based on the fluorescence resonance energy transfer (FRET) between upconversion nanoparticle (UCNP) and gold nanoparticle (AuNP). UCNP and AuNP were linked by a trypsin-sensitive peptide DDDDARC, forming the non-fluorescent UCNP-peptide-AuNP nanosensor. In the presence of trypsin, the peptide was cleaved and the quenched fluorescence was restored; in the presence of trypsin inhibitors , the recovery of the fluorescence was decreased. The nanosensor showed a superb sensitivity and selectivity for trypsin and its inhibitors, with a detection limit of 4.15 ng mL −1 for trypsin. UCNP-peptide-AuNP could eliminate the interference of background fluorescence and avoid the light toxicity, and potentially be used to diagnose trypsin-related diseases or screen trypsin inhibitors.
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ACS Applied Materials & Interfaces
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2017
·
IF 7.504
Lingxiao Lv,Panpan Zhang,Tong Xu,Liangti Qu
Herein, we develop a supersensitive pressure sensor based on a fully air-bubbled ultralight graphene block through a simple sparkling strategy. The obtained sparkling graphene block (SGB) exhibits excellent elasticity even at 95% compressive strain and rebounds a steel ball with an ultrafast recovery speed (∼1085 mm s–1). Particularly, the SGB-based sensor reveals a record pressure sensitivity of 229.8 kPa–1, much higher than other graphene materials, because of the highly cavity-branched internal structure. Impressively, the pressure sensor can detect the extremely gentle pressures even beyond the real human skin and hence are promising for ultrasensitive sensing applications.
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ACS Applied Materials & Interfaces
·
2017
·
IF 7.504
Xiaoqiang Wang,Chao Wang,Meihong Pan,Junting Wei,Fuping Jiang,Rongsheng Lu,Xuan Liu,Yihui Huang,Fang Huang
Taking inspiration from biology’s effectiveness in functionalizing protein-based nanocages for chemical processes, we describe here a rational design of an artificial metalloenzyme for oxidations with the bacterial chaperonin GroEL, a nanocage for protein folding in nature, by supramolecular anchoring of catalytically active hemin in its hydrophobic central cavity. The promiscuity of the chaperonin cavity is an essential element of this design, which can mimic the hydrophobic binding pocket in natural metalloenzymes to accept cofactor and substrate without requiring specific ligand–protein interactions. The success of this approach is manifested in the efficient loading of multiple monomeric hemin cofactors to the GroEL cavity by detergent dialysis and good catalytic oxidation properties of the resulting biohybrid in tandem with those of the clean oxidant of H2O2. Investigation of the mechanism of hemin–GroEL-catalyzed oxidation of two-model substrates reveals that the kinetic behavior of the complex follows a ping-pong mechanism in both cases. Through comparison with horseradish peroxidase, the oxidative activity and stability of hemin–GroEL were observed to be similar to those found in natural peroxidases. Adenosine 5′-triphosphate (ATP)-regulated partial dissociation of the biohybrid, as assessed by the reduction of its catalytic activity with the addition of the nucleotide, raises the prospect that ATP may be used to recycle the chaperonin scaffold. Moreover, hemin–GroEL can be applied to the chromogenic detection of H2O2, which (or peroxide in general) is commonly contained in industrial wastes. Considering the rich chemistry of free metalloporphyrins and the ease of production of GroEL and its supramolecular complex with hemin, this work should seed the creation of many new artificial metalloenzymes with diverse reactivities.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
·
IF 14.7
Qin Xianxian,Li Jiejie,Jiang Tian-Wen,Ma Xian-Yin,Jiang Kun,Yang Bo,Chen Shengli,Cai Wen-Bin
Heterogeneous thermocatalysis of formic acid dehydrogenation by metals in solution is of great importance for chemical storage and production of hydrogen. Insightful understanding of the complicated formic acid dehydrogenation kinetics at the metal-solution interface is challenging and yet essential for the design of efficient heterogeneous formic acid dehydrogenation systems. In this work, formic acid dehydrogenation kinetics is initially studied from a perspective of electrochemistry by decoupling this reaction on Pd catalyst into two short-circuit half reactions, formic acid oxidation reaction and hydrogen evolution reaction and manipulating the electrical double layer impact from the solution side. The pH-dependences of formic acid dehydrogenation kinetics and the associated cation effect are attributed to the induced change of electric double layer structure and potential by means of electrochemical measurements involving kinetic isotope effect, in situ infrared spectroscopy as well as grand canonical quantum mechanics calculations. This work showcases how kinetic puzzles on some important heterogeneous catalytic reactions can be tackled by electrochemical theories and methodologies.
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Scientific Reports
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2017
·Vol. 7
·期 1
·1-9
·
IF 4.259
Wang Tingting,Wu Liqian,Xu Xiaobing,Sun Yuan,Wang Yuanqi,Zhong Wei,Du Youwei
The development of efficient, universal and inexpensive electrocatalysts for hydrogen evolution reaction (HER) is central to the area of sustainable energy conversion. Considering the Co-based sulfides/phosphides have the same catalytic mechanism with the hydrogenases occurring in nature. Here, a new catalyst based on Co 3 S 4 /CoP hybrid that is comprised entirely cheap and earthabundant elements, was first synthesized via a two-step method, the Co(CO 3 ) 0.5 (OH)·0.11H 2 O precursor was prepared by a hydrothermal method, followed by phosphidation and sulphidation under Ar atmosphere simultaneously. The resulting Co 3 S 4 /CoP hybrid material possessed porous core-shell structure with a homogeneous element distribution and large electroactive surface area (~21.04 mF cm −2 ). More importantly, the nanostructured Co 3 S 4 /CoP electrode exhibits excellent HER properties in acid medium with a low onset overpotential of 34 mV, a small Tafel slope of 45 mV dec −1 , as well as a large exchange current density of 150 μA cm −2 . These results obtained in this study indicate that the Co 3 S 4 /CoP hybrid nanorod is promising replacement to the Pt-based catalysts for H 2 production. Moreover, the synthetic method presented in this work can provide an efficient way to synthesis other nanocomposites.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Shijin Wu,Xiaojing Ma,Hongde Yan
The asymmetric reduction of α , β -unsaturated compounds conjugated with electron-withdrawing group by ene-reductases (ERs) is a valuable method for the synthesis of enantiopure chiral compounds. This study introduced an ER from Corynebacterium casei ( Cc ER) which was heterologously expressed in Escherichia coli BL21(DE3), and the purified recombinant Cc ER was characterized for its biocatalytic properties. Cc ER exhibited the highest specific activity at 40 °C and pH 6.5, and showcased appreciable stability below 40 °C over a pH range of 6.0–7.0. The enzyme displayed high resistance to methanol. Cc ER accepted NADH or NADPH as a cofactor and exhibited a broad substrate spectrum towards α , β -unsaturated compounds. It achieved complete conversion of 2-cyclohexen-1-one and good performance for stereoselective reduction of ( R )-carvone (conversion 98 %, diastereoselectivity 96 %). This study highlights the robustness and potential of Cc ER.
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CELL
·
2025
·
IF 42.5
Zhao Yang,Yu-Qi Ping,Ming-Wei Wang,Chao Zhang,Shu-Hua Zhou,Yue-Tong Xi,Kong-Kai Zhu,Wei Ding,Qi-Yue Zhang,Zhi-Chen Song,Ru-Jia Zhao,Zi-Lu He,Meng-Xin Wang,Lei Qi,Christian Ullmann,Albert Ricken,Torsten Schöneberg,Zhen-Ji Gan,Xiao Yu,Peng Xiao,Fan Yi,Ines Liebscher,Jin-Peng Sun
Androgens, such as 5α-dihydrotestosterone (5α-DHT), regulate numerous functions by binding to nuclear androgen receptors (ARs) and potential unknown membrane receptors. Here, we report that the androgen 5α-DHT activates membrane receptor GPR133 in muscle cells, thereby increasing intracellular cyclic AMP (cAMP) levels and enhancing muscle strength. Further cryoelectron microscopy (cryo-EM) structural analysis of GPR133-Gs in complex with 5α-DHT or its derivative methenolone (MET) reveals the structural basis for androgen recognition. Notably, the presence of the “Φ(F/L) 2.64 -F 3.40 -W 6.53 ” and the “F 7.42 ××N/D 7.46 ” motifs, which recognize the hydrophobic steroid core and polar groups, respectively, are common in adhesion GPCRs (aGPCRs), suggesting that many aGPCRs may recognize different steroid hormones. Finally, we exploited in silico screening methods to identify a small molecule, AP503, which activates GPR133 and separates the beneficial muscle-strengthening effects from side effects mediated by AR. Thus, GPR133 represents an androgen membrane receptor that contributes to normal androgen physiology and has important therapeutic potentials.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 6
·2500-2506
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IF 9.931
Fatang Liu,Jingchen Wang,Qinmin Pan
Excellent self-healability is considered as a critical element for next-generation flexible/wearable energy-storage devices. However, realizing superior electrochemical performances remains a big challenge for such devices because self-healability intrinsically offsets their basic energy-storage functions. Here we demonstrate that the conflict can be effectively addressed for a supercapacitor via rationally designing its device configuration at a molecular level. The capacitor is fabricated by in situ integrating polyaniline (PANI) and H2SO4 solution into a single network comprising the copolymer of vinylimidazole and hydroxypropyl acrylate (PVH). The all-in-one configuration combines fast charge-carrier transportation, good structural durability and excellent self-healability. Consequently, the resulting capacitor delivers a high specific areal capacitance and rate capability superior to its counterparts, but also maintains ultra-long cycling life even after breaking/healing 10 times. This example of configuration engineering offers a new and promising avenue to design self-healable energy-storage devices with outstanding performances.
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ChemElectroChem
·
2017
·Vol. 5
·期 4
·659-664
·
IF 4.136
Dawen Yang,Ying Gu,Xu Yu,Zixia Lin,Huaiguo Xue,Ligang Feng
Graphical Cheap and cheerful : Nanostructured Ni 2 P−C was demonstrated as an efficient catalyst for urea electrooxidation. The material exhibited an excellent catalytic ability and was found to display improved charge-transfer kinetics towards urea electrooxidation. Nickel-based materials are a type of cost-effective catalyst for urea oxidation. Herein, we first reported nanostructured Ni 2 P−C as an efficient catalyst for urea electrooxidation. The Ni 2 P−C catalyst was prepared by a facile hydrothermal method and the structure and morphology were further characterized by X-ray diffraction (XRD) and transmission electron microscope (TEM). The hexagonal crystal structure for Ni 2 P was indicated by the characteristic peaks in the XRD patterns, and lattice fringes of Ni 2 P were clearly observed in the high-resolution TEM images. The catalytic ability for urea electrooxidation was studied by cyclic voltammetry and chronoamperometry techniques. It was found that the current density at 0.5 V was ca. 70.4 mA cm −2 , about 2.7 times higher than that of the referenced commercial nickel oxide catalyst. A good catalytic stability for urea oxidation was also obtained. A diffusion-controlled process was observed for urea oxidation on Ni 2 P catalyst while the active sites arising from Ni(II) ion oxidation was following a surface-redox-reaction-controlled process. Kinetics studies by impedance spectroscopy and Tafel slope analysis displayed improved charge-transfer kinetics towards urea electrooxidation. The results demonstrated that Ni 2 P would have potential applications for catalytic urea oxidation.
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RSC Advances
·
2018
·Vol. 8
·期 3
·1427-1435
·
IF 2.936
Zhigang Yi,Juan Wang,Qiong Tang,Tao Jiang
Although many studies have been focused on the photochemistry of antibiotics, the roles of reactive species in photolysis and the effects of dissolved substances on antibiotic photochemical behavior have been poorly examined. The photolytic behaviors of sulfamethazine (SMN) in pure water were investigated via adding different scavengers to quench the active species. Results showed that decomposition of the triplet-excited state of SMN (3SMN*) by direct photolysis was the main path of SMN photolysis in water. Moreover, self-sensitized SMN cannot be ignored during SMN photodegradation. The main photoproducts of SMN were identified by LC-MS/MS, which indicated that SMN could not be mineralized although the photolysis under UV was effective. The effects of Cl−, NO3−, and fulvic acid (FA) (common substances in natural water) on SMN photolytic behaviors were also studied. The triplet-induced halogenation of SMN increases the ionic strength and reduces the ground state SMN; these are the primary causes of promotion of SMN photolysis by Cl−. More ˙OH produced in the presence of NO3− could promote SMN photolysis. Competitive absorption of photons of FA with SMN and ROS scavenged by FA were the main reasons for the inhibition of SMN photolysis. The research findings are helpful for further studies on the environmental risks of ACs in natural waters and promoting the development of AC pollution treatment technology.
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ACS Sensors
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2024
·
IF 8.2
Haining Cui,Jinxin Ma,Youyi Liu,Chan Wang,Qijun Song
In situ and real-time determination of hydroxyl radicals (•OH) in physiological and pathological processes is a great challenge due to their ultrashort lifetime. Herein, an electrochemical method was developed by using dimethyl sulfoxide (DMSO) as a trapping probe for rapid determination of •OH in aqueous solution. When DMSO reacted with •OH, an intermediate product methane sulfinic acid (MSIA) was formed, which can be electrochemically oxidized to methanesulfonic acid (MSA) on the glassy carbon electrode (GCE), resulting in a distinct voltammetric signal that is directly proportional to the concentration of •OH. Other commonly encountered reactive oxygen species (ROS), including hypochlorite anions (ClO–), superoxide anions (O2•–), sulfate radicals (SO4•–), and singlet oxygen (1O2), have showed no interference for •OH determination. Thus, an electrochemical method was developed for the determination of •OH, which exhibits a wide linear range (0.4–5120 μM) and a low limit detection of 0.13 μM (S/N = 3) and was successfully applied for the quantification of •OH in aqueous extracts of cigarette tar (ACT). Alternatively, the same reaction mechanism is also applicable for the determination of DMSO, in which a linear range of 40–320 μM and a detection limit 13.3 μM (S/N = 3) was achieved. The method was used for the evaluation of DMSO content in cell cryopreservation medium. This work demonstrated that DMSO can serve as an electrochemical probe and has valuable application potential in radical study, biological research, and environmental monitoring.
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