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FUEL · 2023 · IF 7.4

Construction of photocatalyst by modification of argentum noble metal and hydrogen doping into WO3 nanoparticles: Enhancing the solar energy utilization

Jun Li,Na Luo,Yinhai Wang,Han Li,Tao Zhang,Xingui Tang,Zhengfa Hu

Solar energy is considered sustainable green energy to prevent environmental pollution. Tungsten trioxide (WO 3 ) is one of the attractive solar energy-driven photocatalysts and photocatalytic supports. Besides, Hydrogen (H) has a small size and can move into many inorganic compounds, and occupy the sites in microstructure as well, with little space structure expansion. H doping in semiconductors attracts more and more attention due to its effect of providing free carriers, resulting in localized surface plasmon resonances which can improve the utilization efficiency of solar energy. In our research, we developed a new method to prepare the H-doped WO 3 whose color turned green, and to prepare Ag/H x WO 3 , which could extend the solar light response range to near-infrared. Furthermore, the photocatalytic activity to degrade RhB solution under UV light and visible light was both improved. The density of free electrons is based on the Drude model to discuss the mechanism of photocatalysis upon the visible. The contact of noble metal Ag and H x WO 3 can play a vital effect in the separation of photogenerated electron-hole pairs. The localized surface plasmon resonances and green coloration bring the tungsten trioxide more remarkable performance together. Results showed that constructed photocatalysis of this work greatly enhanced the utilization rate of solar energy. Photocatalytic for the Degradation of liquid organic pollutants with H x WO 3 is believed to have a bright feature.

CAS / MDL: 7761-88-8 1314-35-8
研究领域: 材料科学 · 环境科学
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Plasmonics · 2020 ·Vol. 15 ·期 6 ·1827-1833 · IF 2.335

Room Temperature Preparation of Surface-Clean Hydrogen-Doped Plasmonic Molybdenum Oxide as a High-Efficient and Degradable Reactive Oxygen Species Scavenger

Wang Junren,Li Hua,Yu Haili,He Yi

Considerable efforts have been made to develop reactive oxygen species (ROS) scavengers for removing high level of ROS. However, most of the reported ROS scavengers are nondegradable and involve harsh reaction conditions as well as utilize various surface ligands. In order to overcome these drawbacks, in the present work, we develop a facile and mild synthesis avenue for preparation of surface-clean hydrogen-doped molybdenum oxide (H 0.34 MoO 3 ) via simply mixing MoO 3 dispersion with aluminum foil under an acidic environment without any surface capping reagents at room temperature. The resulting H 0.34 MoO 3 can act as a broad-spectrum ROS scavenger, including . OH, H 2 O 2 , O 2 − , and 1 O 2 as well as 2, 2-diphenyl-1-picrylhydrazyl (DPPH). The free radical scavenging activity of H 0.34 MoO 3 achieves as high as 71.6% and 99.1% for . OH and DPPH scavenging, which is comparable and superior to that of ascorbic acid that is a classic free radical scavenger. More significantly, the resulting H 0.34 MoO 3 is degrade, which can be degraded into molybdate ions under a neutral environment (pH 7.4).

研究领域: 材料科学 · 生物医学工程
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Nano Research · 2021 ·Vol. 15 ·期 2 ·1288-1294 · IF 8.897

Fine-tuning of Pd-Rh core-shell catalysts by interstitial hydrogen doping for enhanced methanol oxidation

Guo Xiaoyun,Hu Zheng,Lv Jianxin,Li Hui,Zhang Qinghua,Gu Lin,Zhou Wei,Zhang Jiangwei,Hu Shi

Metal catalysts play an important role in the catalytic electrochemical processes and optimization of their performance is usually achieved through alloying with other metal atoms. Doping with interstitial hydrogen atoms is a special but effective way to regulate the electronic structure of host catalysts. Herein we demonstrate the intermixing of Pd and Rh atoms during the hydrogen-doping process of Pd@Rh core-shell nanocubes, forming an alloyed surface in Pd@Rh-H. The catalysts show enhanced performance in electrocatalytic methanol oxidation, as compared to commercial Pt/C and are even better than PdH@Rh core-shell nanocubes. The small structural differences between the two hydride catalysts are revealed by X-ray electron spectroscopy and pair distribution function analysis of electron diffraction. The theoretical calculation results show that Rh in Pd@Rh-H contains more negative charges than Rh in PdH@Rh, indicating more effective charge transfer in Pd@Rh-H. The d-band center ( ε d ) of the Rh site in Pd@Rh-H shifts up, and the synergy between Rh and Pd optimizes the binding energy of CO and OH, inducing preferential catalytic activity. Our work provides guidance for the synthesis of high-performance catalysts by doping with interstitial atoms, which may provide a new strategy to fine-tune the electronic structure of other bimetallic nanoparticles.

研究领域: 催化化学 · 材料科学 · 电化学
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Nano Research · 2021 ·Vol. 15 ·期 4 ·2943-2951 · IF 8.897

Hydrogen-incorporated vanadium dioxide nanosheets enable efficient uranium confinement and photoreduction

Liu Huanhuan,Lei Jia,Chen Jiali,Li Ye,Gong Changyao,Yang Shangjie,Zheng Yamin,Lu Ning,Liu Yan,Zhu Wenkun,He Rong

Photocatalytic reduction of U(VI) represents a novel and effective manner for the removal of U(VI) pollutant from radioactive wastewater. Herein, we successfully incorporated hydrogen into VO 2 nanosheets, which strengthened the interaction between VO 2 and U(VI), thereby achieving a highly active and stable photocatalyst for U(VI) reduction. With the increase of H content in hydric VO 2 (H X -VO 2 ) nanosheets, the bandgap shrank from 2.29 to 1.66 eV, whereas the position of conduction bands remained more negative than the reduction potential of U(VI)/U(IV) (0.41 V vs. NHE). When irradiated by simulated sunlight, the U(VI) removal efficiency over H 0.613 -VO 2 nanosheets reached up to 95.4% within 90 min, which largely outperformed 28.3% of pristine VO 2 nanosheets. The mechanistic study demonstrated that the hydroxylated surface gave rise to the balanced O confinement sites in VO 2 (011), leading to the stabilized adsorption configuration and increased binding strength of UO 2 2+ on H X − -VO 2 nanosheets.

研究领域: 环境科学 · 材料科学
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Chemistry-An Asian Journal · 2018 ·Vol. 13 ·期 6 ·641-647 · IF 3.692

Hydrogen Doping into MoO3 Supports toward Modulated Metal–Support Interactions and Efficient Furfural Hydrogenation on Iridium Nanocatalysts

Lifang Xie,Ting Chen,Hang Cheong Chan,Yijin Shu,Qingsheng Gao

Graphical The straight dope : Controlled hydrogen doping into MoO 3 supports by means of H 2 spillover was introduced to vary the metal–support interactions with Ir, thereby achieving efficient hydrogenation of furfural to furfuryl alcohol under mild conditions (see figure). As promising supports, reducible metal oxides afford strong metal–support interactions to achieve efficient catalysis, which relies on their band states and surface stoichiometry. In this study, in situ and controlled hydrogen doping (H doping) by means of H 2 spillover was employed to engineer the metal–support interactions in hydrogenated MoO x -supported Ir (Ir/H−MoO x ) catalysts and thus promote furfural hydrogenation to furfuryl alcohol. By easily varying the reduction temperature, the resulting H doping in a controlled manner tailors low-valence Mo species (Mo 5+ and Mo 4+ ) on H−MoO x supports, thereby promoting charge redistribution on Ir and H−MoO x interfaces. This further leads to clear differences in H 2 chemisorption on Ir, which illustrates its potential for catalytic hydrogenation. As expected, the optimal Ir/H−MoO x with controlled H doping afforded high activity (turnover frequency: 4.62 min −1 ) and selectivity (>99 %) in furfural hydrogenation under mild conditions ( T= 30 °C, P =2 MPa), which means it performs among the best of current catalysts.

研究领域: 催化化学 · 材料科学
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Journal of Energy Storage · 2024 · IF 8.9

Hydrogen-doping at ambient conditions enhances the pseudocapacitance of H-TiO2@MnO2

Qian Xie,Zhengxin Cai,Zhi Zhang,Yongjun Li,Xinyu Zhang,Jianmin Wang,Jiajia Cai

Deliberate engineering of the excellent skeleton to support the MnO 2 can facilitate electron transfer and charge distribution, contributing to high-energy/power supercapacitance. Herein, an ambient and cost-effective hydrogen-doped method is innovatively employed to prepare H-TiO 2 nanotube arrays (H-TNTAs), where the MnO 2 grows further in situ. After hydrogenation, the capacitance increases by 40-fold, attributing to the improved conductivity. The H-TNTAs supported MnO 2 provides good pseudocapacitive performance, with a specific capacitance of 430.1 F/g at a discharging current of 300 μAcm −2 . The H-TNTAs@MnO 2 coupled active carbon (AC) in 0.5 M Na 2 SO 4 electrolyte is fabricated as the aqueous asymmetric supercapacitor (ASC). The ASC device displays a high energy density of 43.9 Wh kg −1 at a power density of 550 W kg −1 , with an output voltage of 2.2 V and a superior capacitance stability of 86.7 % (over 5000 cycles). The idea for designing the hydrogenated transition metal oxides can be extended to other high-performance metal oxide electrodes for energy storage devices.

研究领域: 材料科学 · 能源存储
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Enhanced capacitance of TiO2 nanotubes topped with nanograss by H3PO4 soaking and hydrogenation doping

Siwei Zhao,Ying Chen,Zhiyang Zhao,Longfei Jiang,Chi Zhang,Jianshou Kong,Xufei Zhu

Anodic TiO 2 nanotubes have been intensively studied for the application in supercapacitors , but the formation of nanograss is often avoided for the belief that it may retard capacitive performance. We fabricate TiO 2 nanotubes topped with nanograss by H 3 PO 4 solution soaking and hydrogenation doping, which in fact increases the capacitance of nanotubes in a fast and convenient way. The new structure exhibits an enhanced areal capacitance by up to 67.7% and by up to 23.5% after 2000 times of cycling. The capacitance generally increases with the nanotube length and reaches the maximum with an optimal nanograss length. The electric charge during hydrogenation doping is determined to quantify the general doping effect. Compared with ordinary nanotubes, nanograss has larger contact area with electrolyte during doping. Therefore, the grass-topped structure yields more electric charge and Ti 3+ during doping, which attributes to the improved capacitance.

研究领域: 材料科学 · 纳米技术 · 电化学 · 能源存储 · 表面工程
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ELECTROCHIMICA ACTA · 2015 · IF 4.504

An Electrochemical Sensor based on p-aminothiophenol/Au Nanoparticle-Decorated HxTiS2 Nanosheets for Specific Detection of Picomolar Cu (II)

Xiaorong Gan,Huimin Zhao,Xie Quan,Yaobin Zhang

An ultrasensitive electrochemical sensor for Cu 2+ detection was first developed based on p-aminothiophenol (PATP) anchored on the surface of Au nanoparticle-decorated hydrogen-incorporated TiS 2 nanosheets (PATP/Au-H x TiS 2 ). In the synthesis process, the plane edges of H x TiS 2 nanosheets offered Au nanoparticles with incubation sites for the heterogeneous nucleation and growth. On the other hand, Au nanoparticles were not only served as an excellent electrical catalyst to facilitate electron transfer and as a substrate for loading PATP molecules by Au-S valent bonds, but also could effectively avoid the aggregation of H x TiS 2 nanosheets . Due to the synergetic effects from Au-H x TiS 2 for signal amplification, the as-formed electrochemical sensor exhibited highly sensitive and selective assaying of Cu 2+ with a detection limit of 90 pM (3σ) and a linear range from 0.2   nM to 5   μM, under optimal conditions. Its specificity was ascribed to the strong coordination interaction between Cu 2+ and N atoms of imine moieties in PATP after electrochemical oxidation .

研究领域: 分析化学 · 纳米科技 · 环境科学
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Science Advances · 2022 ·Vol. 8 ·期 40 · IF 14.957

NIR-photocatalytic regulation of arthritic synovial microenvironment

Bin Zhao,Lingting Zeng,Danyang Chen,Songqing Xie,Zhaokui Jin,Guanglin Li,Wei Tang,Qianjun He

Synovial microenvironment (SME) plays a vital role in the formation of synovial pannus and the induction of cartilage destruction in arthritis. In this work, a concept of the photocatalytic regulation of SME is proposed for arthritis treatment, and monodispersive hydrogen–doped titanium dioxide nanorods with a rutile single-crystal structure are developed by a full-solution method to achieve near infrared–photocatalytic generation of hydrogen molecules and simultaneous depletion of overexpressed lactic acid (LA) for realizing SME regulation in a collagen-induced mouse model of rheumatoid arthritis. Mechanistically, locally generated hydrogen molecules scavenge overexpressed reactive oxygen species to mediate the anti-inflammatory polarization of macrophages, while the simultaneous photocatalytic depletion of overexpressed LA inhibits the inflammatory/invasive phenotypes of synoviocytes and macrophages and ameliorates the abnormal proliferation of synoviocytes, thereby remarkably preventing the synovial pannus formation and cartilage destruction. The proposed catalysis-mediated SME regulation strategy will open a window to realize facile and efficient arthritis treatment.

CAS / MDL: 7439-93-2
研究领域: 生物医学工程 · 材料科学 · 风湿病学
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