ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2023
·Vol. 415
·期 29
·7103-7115
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IF 4.3
Li Guiyin,Li Xinhao,Xu Wenfeng,Li Shennan,Tan Xiaohong,Liang Jintao,Zhou Zhide
1,5-anhydroglucitol (1,5-AG) is of considerable clinical relevance as a biochemical marker of glucose metabolism in the assessment and monitoring of diabetes. Herein, a simple colorimetric biosensor was constructed for the identification and detection of 1,5-AG by using pyranose oxidase (PROD) enzyme cascaded with reduced graphene oxide/persimmon tannin/Pt@Pd (RGO-PT/Pt@Pd NPs) nanozyme. The as-prepared RGO-PT/Pt@Pd NPs had excellent peroxidase-like activity and can be applied as a nanozyme. First, PROD enzyme reacts with the target 1,5-AG, decomposing 1,5-AG into 1,5-anhydrofuctose (1,5-AF) and H 2 O 2 . At this point, the highly catalytic RGO-PT/Pt@Pd NPs nanozyme produces a cascade with PROD enzyme which catalyzes the decomposition of H 2 O 2 to produce O 2 . This in turn oxidizes the substrate 3,3′,5,5′-tetramethylbenzidine (TMB) and produces a color change in the solution. Finally, the detection of 1,5-AG was achieved by measuring the absorption peak at 652 nm with an ultraviolet visible (UV-vis) spectrophotometer. Under optimal conditions, the linear operating range of the 1,5-AG enzyme cascade colorimetric sensor was 1.0–100.0 μg/mL, and the limit of detection (LOD) was 0.81 μg/mL. The proposed colorimetric biosensor was successfully applied to detect 1,5-AG in spiked human serum samples with the recoveries of 97.2–103.9% and RSDs of 1.94–4.48%. It provides a promising developmental assay for clinical detection of 1,5-AG.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Renke Bi,Bing Han,Yijie Shen,Jialong Liu,Zhiyu Wang
Sunlight-driven photocatalytic overall water splitting (OWS) is a promising approach for solar-to-chemical energy conversion. However, its realization with a single photocatalyst by one-step excitation has been extremely limited due to the rapid recombination of photogenerated charges, slow surface redox kinetics, and undesired reverse reactions. Herein, we sought to enhance the OWS performance of SrTiO3 (STO) by exploring the synergistic effects of different kinds of metal/oxide dual cocatalysts. The results show that the Pt/CrOx-STO system had a superior activity, which achieved stoichiometric water splitting with H2/O2 evolution of 1814.17/1020.47 μmol g–1 h–1 under simulated sunlight, without using any sacrificial reagents. The enhanced efficiency can be attributed to the improved interfacial transport of photogenerated charges and the boosted surface kinetics. Importantly, the CrOx layer served as a selective membrane that prevented the O2 diffusion and facilitated H+ transport, while partially covering the highly active site of Pt nanoparticles, thus significantly inhibiting the reverse recombination reaction of H2 and O2. In particular, this dual catalyst system emphasized a low dependence on the properties of the substrate material and is therefore widely applicable and economical. This work demonstrated the potential of the Pt/CrOx dual cocatalyst modification strategy for optimizing photocatalytic OWS, providing a pathway toward selective and sustainable conversion of H2O to H2 and O2.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 43
·19974-19982
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IF 3.3
Hao Fan,Qin Peng,Zhenxing Shen,Xuefeng He,Yiming Yang
Nitric oxide (NO), a major atmospheric pollutant and a precursor to haze, can be removed using the denitration catalyst. Mn and Ni are commonly used as denitration catalyst additives owing to their adsorption abilities for NO and ammonia (NH3). In this study, we synthesized Mn- and Ni-loaded Pt-modified sulfated cerium oxide (PtSCe) catalysts using an impregnation method and explored the effects of these elements. The results revealed that the two elements had contrasting effects on the denitration activity of the catalysts. Mn improved the water vapor and sulfur resistance of the PtSCe sample by increasing the concentration of weak acid sites, enhancing the redox ability, and increasing the content of surface-adsorbed oxygen. The elevation in oxygen vacancies, stimulated by the presence of Ce3+ and Mn3+, swiftly replenished the reactive oxygen species, thereby sustaining the high denitration efficiency of the MnPt/SCe sample. Active sites on the catalyst surface included NH3 adsorbed on Lewis acid sites, NH4+, and –NH2, along with bridging, monodentate, and bidentate nitrate groups. Regarding the catalyst reaction mechanism, we determined that the selective catalyst reduction of NH3-SCR over MnPt/SCe followed both the Eley–Rideal and Langmuir–Hinshelwood mechanisms. These findings offer crucial insights into the intricate relationship between metals, sulfates, and carrier molecules, thus providing implications for future catalyst design.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 40
·18865-18871
·
IF 3.3
Chao Liu,Gang-Gang Chang,Ting-Ting Luo,Yi-Tian Wang,Shi-Tian Xiao,Yao Yao,Hong-Jian Xu,Ge Tian,Christoph Janiak,Hai-Hu Yu,Xiao-Yu Yang
Metal–organic frameworks (MOFs) have great potential for producing photoelectrocatalyzed hydrogen and degrading pollutants, owing to several factors such as high porosity and tunable semiconductor-like properties. Wide band gaps, which restrict their use to only UV light induced reactions, and low efficiencies for the separation of photogenerated charge carriers (electrons and holes) pose significant challenges to the widespread applications of MOFs. In this study, a hierarchical hollow Pt@H-UiO-66-NH2/CdS ternary catalyst was designed and synthesized. The immobilized CdS nanoparticles (NPs) in this catalyst endow the MOF H-UiO-66-NH2 with high visible light absorption ability and the Pt NPs serve as electron sinks to improve charge carrier separation. Furthermore, the hierarchical hollow structure of H-UiO-66-NH2 in the composite contributes to boosting light absorption and shortening the distance for charge transfer. As a proof of principle, Pt@H-UiO-66-NH2/CdS catalyzes methylene blue (MB) degradation with a high rate constant of 1.025 × 10−2 and hydrogen production with a rate of 12 810 μmol g−1 h−1, the latter of which is about 2.3, 11.7 and 173 times higher than those of Pt@UiO-66-NH2/CdS, H-UiO-66-NH2/CdS and Pt@H-UiO-66-NH2, respectively.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 23
·10315-10324
·
IF 3.591
Jianming Fan,Jinhua Xiong,Dayue Liu,Yuanping Tang,Song He,Zhibiao Hu
A novel strategy was developed to fabricate a CdS/Pt photocatalyst (defined as CdS/w%Pt-PAR) via the cathodic photocorrosion effect of CdS. A tentative mechanism for Pt deposition on CdS via the cathodic photocorrosion effect was proposed, based on a series of electrochemical characterization methods, such as cyclic voltammetry and Mott-Schottky tests. Transmission electron microscopy verified that Pt was grafted on the CdS surface via a heterojunction. Moreover, a strong interaction between Pt and CdS was further confirmed by X-ray photoelectron spectroscopy. The optimal photocatalytic H2 evolution rate of CdS/2%Pt-PAR was 1086.1 μmol h−1, 6.4 and 2.6 fold higher than that of the reference samples synthesized by traditional photodeposition (CdS/2%Pt-PD) and chemical reduction (CdS/2%Pt-CR) methods, respectively. Linear sweep voltammetry and fluorescence experiments verified that CdS/2%Pt-PAR has a lower H2 evolution overpotential and faster separation of photogenerated carriers, respectively, compared with CdS/2%Pt-PD and CdS/2%Pt-CR. This work paves a new route for fabricating CdS/metal photocatalysts with highly efficient and stable photocatalytic H2 evolution activity.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Binbin Zhao,Yu Liang,Wenjun Yan,Lei Liu,Jinxiang Dong
Selective hydrogenolysis of biomass-derived glycerol to 1,3-propanediol (1,3-PDO) is of significant industrial value. The conventional synthetic approach for the supported Pt–WOx catalysts with potential for industrial application generally required a high Pt loading with an aim to create more Pt–O–W interfaces owing to the difficulty in controlling the formation of active WOx species and their high dispersion on supports. In this study, a thin coating of a WOx–Ta2O5 solid solution on a Ta2O5 surface was successfully fabricated by the calcination of W-precursor-containing Ta2O5 at a high temperature (i.e., 900 °C), leading to high dispersion of low-polymeric tungsten oxide with abundant oxygen defects on the support surface. The oxygen defects of the WOx species in the WOx–Ta2O5 solid solution layer played a key role in anchoring and dispersing platinum species to maximize the Pt–O–W interface. WOx(900)/Ta2O5-supported Pt exhibits much higher catalytic efficiency toward the production of 1,3-PDO (TOF1,3-PDO = 23.2 g1,3-PDO·gPt–1·h–1) than that of WOx(500)/Ta2O5-containing Pt derived from routine calcination temperatures. Several characterization techniques were applied to examine the state change of WOx on the support by varying the calcination temperature, as well as the effect of WOx species on the dispersion and chemical states of platinum species.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 22
·13080-13086
·
IF 12.732
Mei Zhang,You Xu,Shengqi Wang,Mengying Liu,Lianbang Wang,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
How to boost the electrocatalytic performance of non-Pt catalysts for the hydrogen evolution reaction (HER) to substitute Pt is an important research topic. Herein, by combining a one-pot wet-chemical method and the post surface functionalization, we successfully fabricated polyethylenimine (PEI)-modified bimetallic Au@Rh core–shell mesoporous nanospheres (Au@Rh@PEI MNs). Benefiting from the synergetic effects of Au@Rh core–shell mesoporous architectures and interfacial modification by PEI molecules, the resultant Au@Rh@PEI MNs exhibit excellent electrocatalytic activity and stability for the HER in all pH value solutions, which even surpass the benchmark commercial Pt/C catalyst. Our synthetic protocol may offer guidelines for the rational design of advanced catalysts for water splitting and other electrocatalytic applications.
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Inorganic and Nano-Metal Chemistry
·
2021
·
IF 1.716
Liang Xian,Bi-Quan Su,Yin-Xia Feng,Bei Xi,Zhi-Ying Duan
The hydrolysis of K2[PtCl4] under visible light, the equilibrium, morphology, and size of Pt NPs combined with CDs, the valence states of Pt element and the bonding of Pt NPs with CDs, the influence of different kinds of cyclodextrin (α, β, γ-CDs), the acidity of the solution, and the visible light color on the catalytic ability of Pt NPs were all researched by typical approaches. All results prove visible light irradiation is effectively playing a key role in the reaction process to form Pt NPs in a very narrow size distribution. pH = 9, β-CDs, and purple visible light are the optimized reaction conditions. The Pt-CDs present a high rate constant of 0.88 min−1 in the catalytic reduction of 4-NP. This research is beneficial for expanding photochemical approaches from ultraviolet light to visible light, which is more of green chemistry, low cost, and facile.
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CHEMISTRY OF MATERIALS
·
2020
·
IF 9.567
Sheng-Li Hou,Jie Dong,Zi-Hao Zhu,Liang-Chen Geng,Yue Ma,Bin Zhao
Highly stereoselective hydrogenation of α-pinene under mild conditions in the utilization of natural products is important but challenging. Here, we report a facile strategy for the size-controlled synthesis of ultrafine Pt nanoparticles using a versatile metal–organic cage (Cu-MOC) as a soluble confinement template. The Cu-MOC consists of 12 Cu2(CO2)4 paddlewheel structures, forming a highly symmetric cuboctahedral geometric structure with a cavity of 1.5 nm diameter. Utilizing the space confinement effect of Cu-MOC, the ultrafine Pt nanoparticles can be tuned between 0.88 and 1.35 nm and be highly dispersed in solution. Catalytic investigations indicate that the obtained Pt@Cu-MOC exhibits excellent activity for the hydrogenation of α-pinene to cis-pinane under mild conditions. Both the stereoselectivity and conversion can reach 99%, which are much higher than those of the commercial Pt/C and traditional Pt@PVP catalysts. In addition, this method can also enable other metal to be encapsulated into Cu-MOC, which may bring new inspiration for stereoselective hydrogenation of natural products.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2020
·
IF 16.683
Munir Ahmad,Xie Quan,Shuo Chen,Hongtao Yu,Zhenxing Zeng
Metal sulfide photocatalysts have been leading edge for hydrogen evolution reaction (HER) and solar energy conversion due to their suitable electronic and optical properties. The efficiency of these photocatalysts is mostly restricted by slow transfer of photogenerated holes and sluggish water dissociation kinetics. Here, we proposed HER catalyst comprising of Pt-CrO x sites loaded on ZnCdS nanocrystal (ZnCdS/Pt-CrO x ) that employing a redox couple ( OH/OH − ) transport mechanism to efficiently relay of holes in alkaline media. The Pt sites provide optimal hydrogen adsorption energy and CrO x sites support water dissociation, which speed up water dissociation kinetics and leads to a noticeable enhance in HER (21.1 mmol g −1 h −1 ) and phenol degradation. Such efficient activity could be associated to a better mobility of redox couple and fast water dissociation kinetics in alkaline solution. These types of related works open pathways to generate hydrogen from the sea water, largest water source on earth.
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Nanomaterials
·
2020
·Vol. 10
·期 5
·983
·
IF 4.324
Xueqing Zhu,Hui He,Yanxia Li,Haoyuan Wu,Mingli Fu,Daiqi Ye,Junliang Wu,Haomin Huang,Yun Hu,Xiaojun Niu
Functional metal organic framework (MOF) derivatives have attracted tremendous attention as promising catalysts for various reactions. The thermal decomposition strategies have a vital effect on the structures and physicochemical properties of functional MOF derivatives. Nevertheless, what effect does the pyrolysis strategy have on MOF derivatives need further study. In this work, one-step (under dry air) and two-step (first under N2and then dry air) pyrolysis are chosen to prepare the functional ceria-based MOF derivatives with novel hierarchical pore structure. In comparison with the derivatives prepared by one-step pyrolysis, the two-step pyrolysis composites exhibit better catalytic activity for toluene oxidation due to the higher contents of surface absorbed oxygen species and surface oxygen vacancies. The reusability and durability test demonstrates perfect stability of such functional MOF derivatives. The in-situ UV Raman reveals that two-step strategy is favorable for enhancing the gaseous oxygen activation ability of the functional MOF derivatives. Those findings may instruct the synthesis of functional MOF derivatives via different pyrolysis strategies as well as afford a further understanding of the crucial role of oxygen vacancies.Keywords:metal organic frameworks;functional derivatives;pyrolysis strategies;toluene oxidation;oxygen activation abilities
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Journal of Materials Research and Technology-JMR&T
·
2020
·
IF 5.289
Liang Li,Ya Yang,Yaowei Wang,Manli Liang,Yuanxing Huang
Suitable electrode catalyst is a critical factor for the application of direct methanol fuel cell. In this research, layered double hydroxides (LDH) are chosen as the supporting material for platinum to improve its electrochemical activity, tolerance to carbonaceous intermediates as well as reduce the cost of electrode. Experimental results show that low amount of platinum (42 and 29 mg/g) can be intercalated into the interlayer of LDH with a thickness less than 1 nm, which can effectively enhance the electrochemical activity as well as reduced the cost. Both MgAl-LDH/Pt and NiFe-LDH/Pt have a lower onset potential toward methanol oxidation than commercial 20% Pt/C. In addition, the peak current of NiFe-LDH/Pt is 18.0 mA/cm 2 , which is 1.5- and 4.7-fold higher than that of MgAl-LDH/Pt and commercial 20% Pt/C, respectively. MgAl-LDH/Pt has a higher tolerance to CO poisoning due to its preference to the generation of hydroxyl radical rather than oxygen evolution reaction, which is commonly observed on the surface of NiFe-LDH. By using electrochemical impedance spectroscopy technique, it can be observed that the intercalation of Pt could effectively reduce the electron transfer resistance of LDH.
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