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Advanced Energy Materials · 2017 ·Vol. 7 ·期 18 ·1700700 · IF 16.721

Hydrogenated Core–Shell MAX@K2Ti8O17 Pseudocapacitance with Ultrafast Sodium Storage and Long-Term Cycling

Guodong Zou,Jianxin Guo,Xianyu Liu,Qingrui Zhang,Gang Huang,Carlos Fernandez,Qiuming Peng

Sodium-ion batteries are considered alternatives to lithium-ion batteries for energy storage devices due to their competitive cost and source abundance. However, the development of electrode materials with long-term stability and high capacity remains a great challenge. Here, this paper describes for the first time the synthesis of a new class of core–shell MAX@K 2 Ti 8 O 17 by alkaline hydrothermal reaction and hydrogenation of MAX, which grants high sodium ion-intercalation pseudocapacitance. This composite electrode displays extraordinary reversible capacities of 190 mA h g −1 at 200 mA g −1 (0.9 C, theoretical value of ≈219 mA h g −1 ) and 150 mA h g −1 at 1000 mA g −1 (4.6 C). More importantly, a reversible capacity of 75 mA h g −1 at 10 000 mA g −1 (46 C) is retained without any apparent capacity decay even after more than 10 000 cycles. Experimental tests and first-principle calculations confirm that the increase in Ti 3+ on the surface layers of MAX@K 2 Ti 8 O 17 by hydrogenation increases its conductivity in addition to enhancing the sodium-ion intercalation pseudocapacitive process. Furthermore, the distorted dodecahedrons between Ti and O layers not only provide abundant sites for sodium-ion accommodation but also act as wide tunnels for sodium-ion transport.

研究领域: 材料科学 · 能源存储
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JOURNAL OF BIOMATERIALS APPLICATIONS · 2016 · IF 1.988

Impact of hydrogenation on physicochemical and biomedical properties of pH-sensitive PMAA-b-HTPB-b-PMAA triblock copolymer drug carriers

Feng Xu,Jing-Wen Xu,Yan-Ling Luo

pH-Sensitive poly(methacrylic acid)-block-hydroxyl-terminated polybutadiene-block-poly(methacrylic acid) (PMAA-b-HTPB-b-PMAA) was synthesized and then hydrogenated in this work. The chain structure, phase behavior and thermal properties were characterized by 1H NMR, FTIR, XRD, DSC, TGA, etc., and the physicochemical and biomedical properties were investigated via fluorescence spectroscopy, TEM, DLS, loading and release of drug and MTT, and so on. The experimental results indicated that the hydrogenation led to the change in the chain aggregate structure of hydrophobic HTPB blocks and the formation of more stable spherical core-shell micelle aggregates, and the critical micelle concentration decreased from 41.8 mg L−1 before hydrogenation to 4.4 mg L−1 after hydrogenation. The hydrogenated block copolymer micelle aggregates exhibited pH-triggered response, and could entrap twice as much hydrophobic drug as the unhydrided counterparts and the encapsulation efficiency was significantly improved, which makes them fine to meet the requirements for drug carriers. Therefore, the hydrogenated PMAA-b-HTPB-b-PMAA copolymer micelles as drug target release carriers can be well used in the field of prevention and treatment of cancers.

研究领域: 材料科学 · 生物医学工程 · 药学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2016 · IF 8.328

Enhanced photon-to-electron conversion and improved water resistance of hydrogenated ceria in photocatalytic oxidation at gas–solid interface

Dong Jiang,Wenzhong Wang,Yali Zheng,Ling Zhang

Hydrogenation has been widely employed in solar-driven photocatalysis, to enhance the light absorption and photon-to-electron (PE) conversion of semiconductors. However, there still remain controversies in this field, such as the precise roles of bulk and surface oxygen vacancies (V O ). Furthermore, the influence of hydrogenation on surface reactions in photocatalysis at gas-solid interface has been rarely discussed. Herein, gray CeO 2 was prepared by treating pristine CeO 2 in H 2 /Ar, presenting surface plasma resonance (SPR) like visible light absorption. No modifications on microstructural surface disordering or valence band edge were detected in gray CeO 2 . Hydrogenation induced abundant V O inside both the bulk lattice and the surface layer. Gray CeO 2 presented much enhanced performance as well as improved water resistance in photocatalytic oxidation of gaseous hydrocarbons. Additional post-annealing in air was applied to remove surface V O and discolored the material. With series of characterization including XPS, Raman, EPR and in-situ FTIR, it was found bulk V O mostly contributes to the enhanced PE conversion, while surface V O is mainly responsible for the improved water resistance. Our results unambiguously confirmed hydrogenation as an efficient approach to simultaneously optimize oxide semicomductors in various elementary steps of photocatalysis.

CAS / MDL: 10294-41-4
研究领域: 材料科学 · 环境科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2018 · IF 5.091

Engineering hydrogenated manganese dioxide nanostructures for high-performance supercapacitors

Xiao Ying Liu,Tian Cheng Gong,Jie Zhang,Junyi Ji,Wang Chen Huo,Tong Cao,Yu Xin Zhang,Xianming Zhang,Yunqi Liu

Improving the rate capability of transition metal oxides is of great important for the development of high-performance electrodes for supercapacitors . Here, a novel strategy of hydrogenation to enhance the electron transfer rate of manganese dioxide (MnO 2 ) is proposed. Detailed preparative parameters (i.e. hydrogenation temperature and time) are systematically investigated. The hydrogenated MnO 2 (H-MnO x ) exhibits modified crystal phase/surface structures and increased electrical conductivity . The prepared H-MnO x exhibits high specific capacitance (640 mF cm −2 at current density of 1 mA cm −2 ), good rate capability (89.6% of capacitance retained from 1 to 10 mA cm −2 ), and good cycling stability (84.6% retention after 1000 cycles). The high specific capacitance is ascribed to the unique interconnected ultrathin nanosheets structure, which could not only provide porous channels for electrolyte infiltration to offer sufficient electrode/electrolyte interface, but also shorten the ions diffusion distance inside the active material. The good rate capability could be attributed to the good conductivity of the H-MnO x nanosheets, which was confirmed by the DFT calculation. These results highlight the importance of hydrogenation as a facile yet effective strategy to improve the rate capability of transition metal oxides for supercapacitors.

研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2017 · IF 3.387

Protecting hydrogenation-generated oxygen vacancies in BiVO4 photoanode for enhanced water oxidation with conformal ultrathin amorphous TiO2 layer

Yang Zhang,Xintong Zhang,Dan Wang,Fangxu Wan,Yichun Liu

Introducing appropriate amount of oxygen vacancies by hydrogenation treatment is a simple and efficient way to improve the photoelectrochemical performance of nanostructured oxide photoanodes. However, the hydrogenation effect is often not durable due to the gradual healing of oxygen vacancies at or close to surface of photoanodes. Herein, we tackled the problem by conformal coating the hydrogenated nanoporous BiVO 4 (H-BiVO 4 ) photoanode with an ultrathin layer of amorphous TiO 2 . Photoelectrochemical measurements showed that a 4   nm-thick TiO 2 layer could significantly improve the stability of H-BiVO 4 photoanode for repeated working test, with negligible influence on the initial photocurrent compared to the uncoated one. Mott–Schottky and linear sweep voltammetry measurements showed that donor density and photocurrent density of the H-BiVO 4 electrode almost decayed to the values of pristine BiVO 4 electrode after 3   h test, while the amorphous TiO 2 -coated electrode only degraded by 6% and 5% of the initial values respectively in the same period. The investigation thus suggested that the amorphous TiO 2 layer did protect the oxygen vacancies in H-BiVO 4 photoanode by isolating these oxygen vacancies from environmental oxygen, while at the same time not impeding the interfacial charge transfer to water molecules due to its leaky nature.

CAS / MDL: 18497-13-7 3153-26-2
研究领域: 材料科学 · 能源科学
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ELECTROCHIMICA ACTA · 2016 · IF 4.803

Enhanced photoelectrochemical performance of nanoporous BiVO4 photoanode by combining surface deposited cobalt-phosphate with hydrogenation treatment

Yang Zhang,Dan Wang,Xintong Zhang,Ying Chen,Lina Kong,Peng Chen,Yinglin Wang,Changhua Wang,Lingling Wang,Yichun Liu

Improving charge transportation and interfacial charge transfer in semiconductor photoelectrodes are two critical issues for achieving high-efficiency photoelectrochemical (PEC) water splitting. Herein, a combined hydrogenation treatment and cobalt-phosphate (Co-Pi) deposition is reported to dramatically enhance the PEC performance of nanoporous BiVO 4 photoanode. Linear sweep voltammograms show that after the combined treatment, photocurrent density of nanoporous BiVO 4 photoanode is increased for ca. 3 times at 1.23   V versus reversible hydrogen electrode (RHE), and the onset potential is negatively shifted from 0.53   V to 0.23   V versus RHE. Combined photoluminescence, Mott-Schottky, open circuit potential, as well as electrochemical impedance spectroscopy analyses reveal the synergistic effect of hydrogenation treatment and Co-Pi deposition on enhancing the PEC performance of nanoporous BiVO 4 photoanode, facilitating both charge transportation and interfacial charge transfer without aggravating charge recombination.

研究领域: 材料科学 · 能源科学
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Catalysts · 2025 ·Vol. 15 ·期 9 ·889 · IF 4

Defect Engineering via La Doping and Hydrogenation on Bi4Ti3O12 for Synergistically Enhancing Photocatalytic CO2 to CH3OH

Lijun Xue,Yuxuan Wang,Chenhui Qiu,Hui Wan

Developing highly efficient photocatalysts for CO2reduction remains a great challenge. The large band gap and poor charge carrier dynamics are the major factors limiting the performance of Bi4Ti3O12(BTO). Herein, a series of La-doped Bi4Ti3O12(BLaxTO) nanosheets were synthesized and further modified by NaBH4hydrogenation to create surface defect-rich H-BLaXTO nanosheets. Characterizations and theoretical calculations confirmed that the synergistic effect of La doping and hydrogenation significantly enhanced visible-light absorption, promoted charge separation, and improved the electron reduction capacity. When applied to photocatalytic CO2reduction, the H-BLa0.2TO catalyst achieved a superior CH3OH production rate of 7.90 μmol·g−1·h−1, which is 5.6 times higher than that of pristine Bi4Ti3O12. Moreover, the H-BLa0.2TO catalyst maintained excellent stability over four consecutive cycles. This study offers an integrated strategy for constructing high-performance bismuth-based photocatalysts through elemental doping and defect engineering.

研究领域: 材料科学 · 光催化 · 环境化学 · 能源化学 · 纳米材料 · 表面科学
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Ferromagetic-paramagnetic transformation in hydrogenated ferrous titanate

Jinming Shi,Yue Chang,Yuanshun Tang,Xuanbo Wang,Wenqing Yao,Zhenxing Yue,Badar Minhas,Jiangli Cao

Abstarct Ferrous titanate (FeTiO 3 ) nanoparticles with hexagonal disc structure were prepared by a simple hydrothermal method . The VSM results show that ferromagnetic-paramagnetic transition of FeTiO 3 caused by high temperature hydrogenation. The morphology and lattice structure of FeTiO 3 was characterized in detail by XRD , Raman, SEM and TEM . It was found that the magnetic transition of FeTiO 3 nanoparticles after hydrogenation could be attributed to the change of lattice structure and surface effect. Further research by XPS found that the high temperature hydrogenation treatment could cause the change of elemental valence states and oxygen vacancies concentration for FeTiO 3 . The weakening of double exchange interaction (Fe 2+ -O-Fe 3+ ) and the reduction of uncompensated surface spin were the main cause of the ferromagnetic-paramagnetic transition. This experiment would provide a new idea for regulating the magnetic property of materials.

研究领域: 材料科学 · 物理学
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2016 ·Vol. 19 ·期 4 ·2961-2973 · IF 4.449

One-step hydroprocessing of fatty acids into renewable aromatic hydrocarbons over Ni/HZSM-5: insights into the major reaction pathways

Shiyou Xing,Pengmei Lv,Jiayan Wang,Junying Fu,Pei Fan,Lingmei Yang,Gaixiu Yang,Zhenhong Yuan,Yong Chen

For high caloricity and stability in bio-aviation fuels, a certain content of aromatic hydrocarbons (AHCs, 8–25 wt%) is crucial. Fatty acids, obtained from waste or inedible oils, are a renewable and economic feedstock for AHC production. Considerable amounts of AHCs, up to 64.61 wt%, were produced through the one-step hydroprocessing of fatty acids over Ni/HZSM-5 catalysts. Hydrogenation, hydrocracking, and aromatization constituted the principal AHC formation processes. At a lower temperature, fatty acids were first hydrosaturated and then hydrodeoxygenated at metal sites to form long-chain hydrocarbons. Alternatively, the unsaturated fatty acids could be directly deoxygenated at acid sites without first being saturated. The long-chain hydrocarbons were cracked into gases such as ethane, propane, and C6–C8 olefins over the catalysts' Brønsted acid sites; these underwent Diels–Alder reactions on the catalysts' Lewis acid sites to form AHCs. C6–C8 olefins were determined as critical intermediates for AHC formation. As the Ni content in the catalyst increased, the Brønsted-acid site density was reduced due to coverage by the metal nanoparticles. Good performance was achieved with a loading of 10 wt% Ni, where the Ni nanoparticles exhibited a polyhedral morphology which exposed more active sites for aromatization.

CAS / MDL: 110-82-7
研究领域: 能源化学 · 催化化学
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Nature Communications · 2022 ·Vol. 13 ·期 1 ·1-12 · IF 17.694

Hydrogenated Cs2AgBiBr6 for significantly improved efficiency of lead-free inorganic double perovskite solar cell

Zhang Zeyu,Sun Qingde,Lu Yue,Lu Feng,Mu Xulin,Wei Su-Huai,Sui Manling

Development of lead-free inorganic perovskite material, such as Cs 2 AgBiBr 6 , is of great importance to solve the toxicity and stability issues of traditional lead halide perovskite solar cells. However, due to a wide bandgap of Cs 2 AgBiBr 6 film, its light absorption ability is largely limited and the photoelectronic conversion efficiency is normally lower than 4.23%. In this text, by using a hydrogenation method, the bandgap of Cs 2 AgBiBr 6 films could be tunable from 2.18 eV to 1.64 eV. At the same time, the highest photoelectric conversion efficiency of hydrogenated Cs 2 AgBiBr 6 perovskite solar cell has been improved up to 6.37% with good environmental stability. Further investigations confirmed that the interstitial doping of atomic hydrogen in Cs 2 AgBiBr 6 lattice could not only adjust its valence and conduction band energy levels, but also optimize the carrier mobility and carrier lifetime. All these works provide an insightful strategy to fabricate high performance lead-free inorganic perovskite solar cells.

研究领域: 材料科学 · 能源科学
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ACS Applied Nano Materials · 2018 · IF 0

Green and Sensitive Flexible Semiconductor SERS Substrates: Hydrogenated Black TiO2 Nanowires

Lili Yang,Yusi Peng,Yong Yang,Jianjun Liu,Zhiyuan Li,Yunfeng Ma,Zhang Zhang,Yuquan Wei,Shuai Li,Zhengren Huang,Nguyen Viet Long

Hydrogenation was discovered to be an effective method to improve the surfaced-enhanced Raman scattering (SERS) performance of semiconductor TiO2 and enhance its enhancement factor (EF) by at least 3 orders of magnitude. The TiO2 substrate hydrogenated for 3 h showed the most remarkable SERS activity with a detection limit of 1 × 10–7 M for R6G and an EF of 1.20 × 106, which can be comparable to the Ag substrate. The remarkable SERS activities can be attributed to the chemical enhancement mechanism dominated by the enhanced photoinduced charge transfer (PICT) process between R6G and the oxygen vacancy-containing partly amorphous black TiO2 NWs substrate, as well as the electromagnetic enhancement (EM) derived from the metal-like local surface plasma resonance (LSPR) of the hydrogenated randomly oriented TiO2 nanowires. The first principle based on the density functional theory has been applied to demonstrate the appearance of tailed electron energy state produced by hydrogenation and provide the reasonable explanation for an easier PICT process, a stronger light absorption, and the enhanced SERS performance of our hydrogenated TiO2 substrates. Another impressive fact was that the photodegradation capability of TiO2 was also evidently improved. After 14 cycles of detection-and-degradation of R6G molecules, the substrates can still maintain regenerative and remarkable SERS activity. Ultrasensitive SERS activity and self-cleaning performance were successfully integrated on the black TiO2 NWs substrate by hydrogenation. Moreover, our substrate exhibited the excellent signal reproducibility and the outstanding stability of antioxidation in atmosphere thanks to the protection of the surface amorphous layer.

研究领域: 材料科学 · 光催化 · 分析化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2017 · IF 9.446

Scalable preparation of defect-rich free-standing TiO2 sheets with visible-light photocatalytic activity

Hanyang Gao,Guoxin Hu,Juan Sui,Chao Mu,Wenfeng Shangguan,Min Kong,Wei Shentu

In this research, two interesting phenomena were reported and analyzed: First, two-dimensional tiny titania nanoplates (4–5 nm lateral size, 0.4–0.5 nm thickness) with rich edge-defects were found to self-assemble into free-standing thin sheets with large lateral size in a freeze-drying process with the aid of linker; Second, when subjected to a moderate hydrogenation treatment, these self-assembled sheets could be crystallized into integral anatase sheets while the edge-defects of the building blocks were maintained on the surface or inside the body of the crystal and the flexible sheet-like shape were also maintained. Based on these observations, a method for scalable preparing free-standing defect-rich TiO 2 with a two-dimensional sheet-like morphology was proposed. The defects (oxygen vacancies) endowed the TiO 2 a grayish-black color and visible-light responsibility. By using the dispersion of these defect-rich anatase sheets, a film could be densely deposited on flexible substrates in a layered structure and showed an efficient performance in acetaldehyde decomposition under the irradiation of visible light. Since it has always been a technical challenge to prepare crystallized visible-light-driven TiO 2 films on plastic substrates with a low heat tolerance, this work may also provide a new approach to this problem.

CAS / MDL: 13463-67-7
研究领域: 材料科学 · 环境科学
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