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Journal of Physical Chemistry Letters · 2023 · IF 5.7

Single-Molecule Force Spectroscopy of Deoxyribonucleic Acid and Deoxyribonucleic Acid Polymerase Activity Impacted by Alkylating Agents

Tianyu Cai,Jiaqing Zhang,Jingjing Deng,Qinman Tian,Ruoqi Zhang,Haokai Geng,Yuedong Liu,Keding Zhong,Liting Wen,Chunxiang Liu,Xun Hu,Yuehui Li,Zhipeng Li,Shipeng Hao,Kai Yang,Huizhong Xu

DNA alkylating agents are widely used in anticancer pharmacology. Although shown to induce cross-linking and/or methylation of DNA, how they affect the mechanical properties of DNA and activity of DNA enzymes remains to be elucidated. Here, we perform single-molecule optical tweezer experiments on DNA treated with alkylating agents, including melphalan, cisplatin, and dacarbazine. While all three drugs induce a significant increase of overstretching force and a reduction of hysteresis, suggesting stabilization of DNA against shearing forces, their effects on elasticity of DNA were quite different, with the largest change in persistence length induced by cisplatin. Furthermore, we find that these alkylating-agent-induced changes on DNA have different effects on processivity of DNA polymerase, with melphalan and cisplatin showing significantly reduced activity and dacarbazine showing little effect. Overall, our results provide new insights into the effects for these alkylating agents, which could potentially facilitate a better design of related drugs.

研究领域: 生物化学 · 生物物理 · 分子生物学 · 药理学 · 癌症研究
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2018 · IF 3.141

Construction of Nanoreactors Combining Two-Dimensional Hexagonal Boron Nitride (h-BN) Coating with Pt/Al2O3 Catalyst toward Efficient Catalysis for CO Oxidation

Wei Bi,Yanjie Hu,Wenge Li,Hao Jiang,Chunzhong Li

In this work, a nanoreactor combining layers of facile traditional two-dimensional (2D) material, hexagonal boron nitride (h-BN, which often called the white graphene) with Pt/Al2O3 catalyst was designed to exhibit higher stability, activity, and selectivity in automobile exhaust treatment. Characterization revealed that h-BN does coat on the surface of platinum and forms a distinct Pt@h-BN/Al2O3 core–shell nanostructure. This as-prepared catalyst possesses good thermal stability and selectivity, because of the excellent high-temperature tolerance and the multidefected structure of the h-BN shell; that is, small molecules such as CO and O2 can easily intercalate into the nanoreactor, while large molecules such as propylene are blocked out. Meanwhile, the intercalated reactants can achieve the conversion of CO to CO2 faster (ΔT100 = 20 °C) with the confinement effect. The study indicates that constructing a nanoscale confined environment with two-dimensional (2D) coating can enhance the performance of the catalyst in multiple aspects and simultaneously provide a good example for designing nanostructured catalysts with multifaceted improvement.

研究领域: 催化化学 · 纳米材料科学 · 环境催化 · 能源化学 · 表面科学
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Energy & Environmental Materials · 2020 ·Vol. 4 ·期 4 ·596-602 · IF 0

Platinum-Induced Pseudo-Zn-Air Reaction Massively Increases the Electrochemical Capacity of Aqueous Zn/V5O12·6H2O Batteries

Gongzheng Yang,Chengxin Wang

How to effectively improve Zn 2+ -storage properties is now becoming an urgent issue in the development of high-energy-density aqueous zinc-ion batteries. Here, a new method is proposed to massively increase the electrochemical capacity of aqueous Zn/V 5 O 12 ·6H 2 O batteries. By adding a small amount of platinum (Pt, 1.5 wt.%) and keeping other factors constant, the V 5 O 12 ·6H 2 O-Pt electrodes deliver a much higher specific capacity (440 mAh g −1 at 500 mA g −1 ) than do V 5 O 12 ·6H 2 O electrodes (270 mAh g −1 at 500 mA g −1 ). The structural and morphological evolution of V 5 O 12 ·6H 2 O during cycling results in Zn 2+ ion insertion/extraction and the formation/disappearance of the zinc hydroxyl complex (Zn 4 SO 4 (OH) 6 ∙5H 2 O, ZHS), where the latter is closely related to the surface redox reaction, promoting Zn 2+ ion stripping/plating on the Zn anode and consequently leading to extra electron transfer. Electrochemical tests in the absence of oxygen reveal that the Pt additive has no contribution and is even counterproductive to electric conductivity but favors remarkable enhancement of the pseudocapacitance. Accordingly, it is apparent that a strong causal relationship exists between Pt and the ZHS. In consideration of the catalytic application for oxygen reduction, Pt is expected to play a vital role in enhancing the electrochemical capacity through the pseudo-Zn-air reaction. This finding introduces a new strategy for achieving high-performance aqueous zinc-ion batteries.

研究领域: 电化学 · 能源材料 · 无机化学 · 储能技术 · 纳米材料科学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2016 ·Vol. 23 ·期 10 ·10050-10057 · IF 2.76

Hydrothermal electrocatalytic oxidation for the treatment of herbicides wastewater

Xiao Hanshuang,Lv Baoying,Gao Junxia,Zhao Guohua

A hydrothermal electrocatalytic oxidation (HTECO) method is adopted to treat the biorefractory and toxic 2,4-dichlorophenoxyacetic acid (2,4-D) herbicides wastewater on nano-Pt/Ti electrode in the existence of H 2 O 2 . Comparisons for the removal of 2,4-D and total organic carbon (TOC) have been carried out between HTECO with individual electrochemical oxidation (EO) and hydrothermal catalytic oxidation (HTCO), showing that high mineralization efficiency was obtained in HTECO process. The possible factors resulting in the high removal efficiency in HTECO process have been studied by investigating the properties of the electrode and solution in hydrothermal condition, the amount of active radicals, the decay kinetic, and evolution of main intermediates of 2,4-D. Thus, an enhanced mechanism for HTECO method for the treatment of herbicides wastewater has been obtained.

研究领域: 环境工程 · 电化学工程 · 水污染控制 · 高级氧化技术 · 环境催化 · 污染物降解动力学
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Journal of Nanomaterials · 2018 ·Vol. 2018 ·期 1 ·1465760 · IF 2.207

Synthesis of Platinum Nanocrystals within Iodine Ions Mediated

Jiamao Li,Jingwei Hou,Yu Gong,Chengjian Xiao,Lei Yue,Linjie Zhao,Huan Ma,Heyi Wang,Shuming Peng,Chao Chen,Hongli Chen

A liquid-phase reducing method of synthesizing Pt nanocrystals was demonstrated, and dendrite-, cube-, and cuboctahedron-shaped Pt nanocrystals (NCs) with well-defined monomorphic were successfully synthesized through iodine ions mediated with the CTAB agent. When the KI concentration was increased to thirty times of K 2 PtCl 4 at the nucleation stage, the high-quality Pt nanodendrites could be obtained. However, no matter how many KI were added at the growth age, only cube- and cuboctahedron-shaped Pt nanocrystals formed. The results of high-resolution TEM, EDX, and XRD indicated that the size and shape of Pt NCs could be turned by changing the concentration and time of KI. In the nucleation stage, it might be due to that some iodine ions adsorb on the surfaces of Pt NCs, which probably cause the rapid growth process resulting in the formation of Pt nanodendrites. In the growth stage, although high concentrations of I − ions could contribute to the shape control and generate bigger particles of Pt NCs, small Pt particles do not grow into dendrites. The insight into the role of I − ions in synthesis of Pt NCs reported here provided a viewpoint for clearly understanding the formation mechanism of anisotropic platinum nanostructures.

研究领域: 纳米材料科学 · 物理化学 · 无机合成 · 催化化学 · 材料表征技术
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Journal of CO2 Utilization · 2017 · IF 4.292

A green process for production of p-aminophenol from nitrobenzene hydrogenation in CO2/H2O: The promoting effects of CO2 and H2O

Lijun Zhao,Haiyang Cheng,Tong Liu,Yan Li,Zhong Ying,Wenjing Yang,Weiwei Lin,Xiangchun Meng,Chengxue Wang,Fengyu Zhao

An efficient green process was developed for production of p -aminophenol (PAP) from hydrogenation of nitrobenzene (NB) over a traditional Pt/Al 2 O 3 catalyst in a reaction medium of supercritical CO 2 (scCO 2 ) and H 2 O without any additional acid catalyst involved. The combination of scCO 2 and H 2 O was confirmed to be effective for the production of PAP. The acidity, aroused by the in situ formed carbonic acid, increased with CO 2 pressure, which acted as acid catalysis during the reaction, and it can easily self-neutralize by depressurization of CO 2 , resulting in a green and a intensive process for it removed the final neutralization and salts disposal of the traditional liquid acids. Under the optimal reaction conditions, a high yield to PAP (68.9%) was achieved at the high conversion of NB (98.5%). Moreover, the results of in situ diffuse reflectance FTIR spectra revealed that CO was generated by the reverse water-gas shift reaction (CO 2   +   H 2   →   CO   +   H 2 O), it can adsorbed on the surface of Pt/Al 2 O 3 to suppress the undesired deep hydrogenation of N -phenylhydroxylamine (PHA) to aniline (AN), which also contributed to the obtained high selectivity of PAP. Therefore, the present green and efficient catalysis process will arouse the interest of researchers in the fields of the green and sustainable organic synthesis.

研究领域: 绿色化学 · 有机合成 · 催化化学 · 环境友好工艺 · 工业化学
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Journal of Materials Chemistry A · 2013 ·Vol. 1 ·期 13 ·4228-4235 · IF 0

Activation of specific sites on cubic nanocrystals: a new pathway for controlled epitaxial growth towards catalytic applications

Yu Bai,Ran Long,Chengming Wang,Ming Gong,Yanrui Li,Hao Huang,Hui Xu,Zhengquan Li,Mingsen Deng,Yujie Xiong

A method has been developed for controlled epitaxial growth on cubic nanocrystals by selectively activating their surface via etching. For example, it produces Pd concave nanocubes via seeding growth on their corners and edges, and in turn, formulates highly active sites for catalysis. This method offers a better capability of preventing atomic addition on undesired locations and maintaining particle size in the seeding process, as compared with the previous technique. With the particle size well maintained, the products fully exhibit superior electrocatalytic performance enabled by active sites and high-index facets in formic acid oxidation. Another contribution of this work is to enable the growth of a noble metal with high catalytic activities on another type of cheaper metal, which greatly reduces the usage of expensive materials while retaining high catalytic activity. In this article, we have demonstrated the deposition of a very limited amount of Pt (only 3.3 wt%) on Pd nanocrystals towards high electrocatalytic activities in an oxygen reduction reaction. Preliminary studies demonstrate that the synthetic strategy can be also applied to the controllable deposition of a different material on the faces of a nanocrystal by simply altering surface conditions.

研究领域: 材料化学 · 纳米科学与技术 · 催化化学 · 电化学 · 表面科学 · 功能纳米材料
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Size-modulated Pt nanoparticles for low-temperature plasmon-enhanced hydrogen production from aqueous phase reforming of methanol

Naiwei Fu,Ruiyi Wang,Xianmo Gu,Yunwei Wang,Jun Ren,Zhanfeng Zheng

Al 2 O 3 supported Pt nanoparticles photocatalyst enables efficient hydrogen production (115.2 μmol min −1  g cat −1 ) through aqueous phase reforming of methanol (APRM) reaction under light irradiation at low temperatures of 150 °C, which is 6 times higher than that of APRM reaction conducted in the dark. We demonstrate that the particle size of Pt nanoparticles greatly affected the light absorption ability, which is of great importance for light utilization of the photocatalyst. The medium particle size of Pt nanoparticles enables the lower electron density states, which is benefit for the dehydrogenation of methanol and the sequential water–gas shift (WGS) reaction and eventually promoted the photocatalytic performance for hydrogen production.

研究领域: 催化 · 纳米技术 · 能量转换 · 光催化 · 化学反应工程
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CHINESE JOURNAL OF CATALYSIS · 2017 · IF 2.813

La-doped Pt/TiO2 as an efficient catalyst for room temperature oxidation of low concentration HCHO

Honggen Peng,Jiawei Ying,Jingyan Zhang,Xianhua Zhang,Cheng Peng,Cheng Rao,Wenming Liu,Ning Zhang,Xiang Wang

Catalytic oxidation of formaldehyde (HCHO) is the most efficient way to purify indoor air of HCHO pollutant. This work investigated rare earth La-doped Pt/TiO 2 for low concentration HCHO oxidation at room temperature . La-doped Pt/TiO 2 had a dramatically promoted catalytic performance for HCHO oxidation. The reasons for the La promotion effect were investigated by N 2 adsorption, X-ray diffraction, CO chemisorption , X-ray photoelectron spectroscopy, transmission electron microscopy (TEM) and high-angle annular dark field scanning TEM . The Pt nanoparticle size was reduced to 1.7 nm from 2.2 nm after modification by La, which led to higher Pt dispersion, more exposed active sites and enhanced metal-support interaction. Thus a superior activity for indoor low concentration HCHO oxidation was obtained. Moreover, the La-doped TiO 2 can be wash-coated on a cordierite monolith so that very low amounts of Pt (0.01 wt%) can be used. The catalyst was evaluated in a simulated indoor HCHO elimination environment and displayed high purifying efficiency and stability. It can be potentially used as a commercial catalyst for indoor HCHO elimination.

研究领域: 环境催化 · 材料化学 · 纳米科学 · 大气污染控制 · 表面化学 · 多相催化
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

High-temperature flexible heat flux sensors

Yong Huang,Lida Xu,Qibin Zhuang,Xiong Zhou,Zhenjin Xu,Wei Xiao,Xin Liu,Qinnan Chen,Yang Zhao,Chao Wu,Daoheng Sun,Dezhi Wu

High-temperature heat flux sensors play a pivotal role in detecting the dynamic heat exchange processes of heating and cooling, in high-temperature environments. However, the detection of surface heat flux on curved parts operating at high temperatures remains a formidable challenge. Flexible thin-film heat flux sensors, while offering benefits such as conformal adhesion and excellent portability, are typically limited by low operational temperatures and narrow measurement ranges. This work proposes a high-temperature flexible heat flux sensor based on multi-layered high-temperature resistant ceramics nanofibre membranes that one layer worked as a substrate and the other two work as thermal resistance layers, and direct ink writing platinum sensitive elements with Wheatstone Bridge configuration. The prototype sensor is capable of quantifying heat flux reaching 1330 kW/m 2 and withstands temperature as high as 1200 °C. The sensor is bendable with resistance change only about 0.5 % even when the bending radius was larger than 10 mm. These extraordinary characteristics indicate that such methodology will offer a new way for the development of high-temperature thin-film flexible heat flux sensors, demonstrating considerable potential for applications in high-temperature environments.

研究领域: 传感器技术 · 材料科学 · 热物理学 · 仪器仪表工程 · 高温测量技术
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2018 · IF 11.698

Anchoring ultrafine Pt electrocatalysts on TiO2-C via photochemical strategy to enhance the stability and efficiency for oxygen reduction reaction

Jingyu Wang,Min Xu,Jianquan Zhao,Huaifang Fang,Qingzhu Huang,Weiping Xiao,Tao Li,Deli Wang

The activity and stability of Pt electrocatalysts are crucial issues for energy conversion systems involving oxygen reduction reaction (ORR). In this work, the ultrafine Pt nanoparticles were in situ reduced by the photogenerated electrons on TiO 2 surface so that most of them selectively anchored around the TiO 2 nanocrystals. The presence of well-dispersed TiO 2 on carbon surface strengthened the metal-support interaction, giving rise to the improved ORR catalytic activity with ∼49 mV positive shift of half-wave potential as compared to commercial 20 wt% Pt/C. More importantly, the Pt/TiO 2 -C catalysts exhibited a more durable performance after 10,000 cycles in terms of the decrease in electrochemical surface area (0.8%) and mass activity (0.9%), much lower than those of Pt/C (10.2% and 33.3%). The high-temperature durability test also revealed a much higher retention of ORR activity. The results demonstrated that anchoring Pt on well-dispersed TiO 2 -decorated carbon would be an effective strategy to enhance the ORR performance by strong metal-support interaction, which facilitated the electron transfer during catalytic reactions as well as prevented Pt aggregation during durability test.

研究领域: 电催化 · 能源转换 · 纳米材料 · 表面科学 · 物理化学 · 材料化学
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Science Advances · 2022 ·Vol. 8 ·期 44 · IF 14.957

Identification of the active triple-phase boundary of a non-Pt catalyst layer in fuel cells

Yu-Cheng Wang,Wen Huang,Li-Yang Wan,Jian Yang,Rong-Jie Xie,Yan-Ping Zheng,Yuan-Zhi Tan,Yue-Sheng Wang,Karim Zaghib,Li-Rong Zheng,Shu-Hui Sun,Zhi-You Zhou,Shi-Gang Sun

The rational design of non-Pt oxygen reduction reaction (ORR) catalysts and catalyst layers in fuel cells is largely impeded by insufficient knowledge of triple-phase boundaries (TPBs) in the micropore and mesopore ranges. Here, we developed a size-sensitive molecular probe method to resolve the TPB of Fe/N/C catalyst layers in these size ranges. More than 70% of the ORR activity was found to be contributed by the 0.8- to 2.0-nanometer micropores of Fe/N/C catalysts, even at a low micropore area fraction of 29%. Acid-alkaline interactions at the catalyst-polyelectrolyte interface deactivate the active sites in mesopores and macropores, resulting in inactive TPBs, leaving micropores without the interaction as the active TPBs. The concept of active and inactive TPBs provides a previously unidentified design principle for non-Pt catalyst and catalyst layers in fuel cells.

研究领域: 燃料电池 · 催化 · 材料科学 · 电化学 · 纳米技术
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