DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 8
·3467-3477
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IF 3.3
Wenhui Hu,Zhongxin Song,Lingna Sun,Lei Zhang,Qianling Zhang,Xiangzhong Ren,Yongliang Li
Efficient separation of photogenerated charge carriers is essential for maximizing the photocatalytic efficiency of semiconductor materials in oxygen evolution reactions (OER). This study presents a novel trimetallic photocatalyst, MIL-100(Fe)/TiO2/CoOx, synthesized through a facile microwave-assisted hydrothermal method followed by atomic layer deposition (ALD). The porous MIL-100(Fe) serves as a support for the sequential deposition of TiO2 and CoOx layers via ALD, which enhances electron–hole pair separation and minimizes their recombination. Characterization using transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) confirms the uniform deposition of TiO2 and CoOx layers on the MIL-100(Fe) surface. The optimized photocatalyst, processed with 20 deposition cycles of Co, exhibits exceptional photocatalytic OER performance, with an oxygen evolution rate of 558.3 μmol g−1 h−1. This enhancement in activity is attributed to the synergistic interaction between the spatially separated TiO2 and CoOx cocatalysts, which facilitates efficient charge transfer and increases the number of active sites. These findings highlight the potential of ALD-fabricated heterostructures in the development of advanced photocatalysts for sustainable energy production.
研究领域:
材料科学
·
能源化学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 9
·期 3
·1678-1691
·
IF 11.301
Fang F. Wang,Chang D. Chen,Wei Wang,Ming L. Kang,Ying Gao,Xue B. Chen,Jing Zhang
Different from transition metals, Na ions cannot be incorporated in the WO3 lattice, but exist in the open framework formed by corner-sharing WO6 octahedra. Based on this channel-inserted Na-doping mechanism, herein, an in situ ion migration-based internal electric field (IEF) engineering strategy is developed. Firstly, Na channel-doped WO3 (Na/WO3) was prepared via a hydrothermal method. Driven by an increase in temperature, Na ions directionally migrated through channels towards the surface region of WO3, leading to an uneven charge distribution between the inner and outer side of the WO3 structure, together with the formation of a core–shell m-WO3/h-WO3 phase junction, and then the IEF from h-WO3 (+) to m-WO3 (−) was built. With a further increase in temperature, Na ions formed chemical bonds with O atoms belonging to the WO6 octahedra, forming a series of core/shell heterojunctions with consecutive –O–W–O– at the interface, including m-WO3/T-Na2W4O13 and m-WO3/T-Na5W14O44, which provide a pathway for the electron transfer. The distinct O 1s oxidation states between the two sides of the atomic junction interface were suggested to be the driving force for the formation of IEF in two heterojunctions. Electrons transfer to one side with a higher O 1s oxidation state along –O–W–O– bands at the interface to build IEF. Transient photocurrent measurement, photoluminescence spectroscopy, steady-state surface photovoltage spectroscopy (SS-SPV) and Mott–Schottky curves were used to investigate separation efficiencies of Na/WO3-T and the relationship with their relative IEF strength and activities. Results indicate that the synergistic effect of IEF and junctions is the main reason for the efficient carrier separation, finally resulting in improved photocatalytic oxygen evolution.
研究领域:
材料科学
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化学工程
·
能源科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Fangxia Xie,Qing Xi,Mei Zhang,Rui Li,Xiaoming Gao,Houfen Li,Xiaochao Zhang,Yawen Wang,Yunfang Wang,Xiuping Yue,Jianxin Liu,Caimei Fan
Directing the transfer of photoinduced charges to various reaction sites through catalyst design plays crucial roles in enhancing photocatalytic oxygen evolution. Herein, we used a facile alcoholysis method to synthesize amorphous FeOOH modified light-switchable oxygen vacancies BiOBr, which exhibited outstanding photocatalytic oxygen evolution activity. Density functional theory calculations, photoelectronchemical tests and kelvin probe force microscopy revealed that FeOOH overlayer acts as the hole storage layer, while oxygen vacancies (OVs) provided a number of electron trap centers. Benefiting from this synergistic effect, the photogenerated charges showed an outstanding directional transfer performance, which greatly prolong the lifetime of the photo-induced charge carriers. Moreover, as a cocatalyst for water oxidation, FeOOH can effectively lower the kinetics barriers and provide more active sites for oxygen evolution reaction. Therefore, under simulated sunlight irradiation, the 2%FeOOH/BiOBr photocatalyst demonstrated remarkable photocatalytic activity towards oxygen evolution, achieving a rate of 284.34 μmol·g −1 ·h −1 , which is around 1.71 folds than pure BiOBr. Finally, the possible reaction mechanism has also been discussed. This work has provided valuable insights and inspiration for the effective design and optimization of BiOBr-based catalysts, which play a critical role in facilitating efficient directional transfer of photogenerated charges.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Ran Wang,Yawei Wang,Shufang Chang,Shu Jin,Yinlin Shao,Xiaoxiang Xu
Complete solid solutions between LaTaON 2 and SrZrO 3 , i.e. (LaTaON 2 ) 1−x (SrZrO 3 ) x (0 ≤ x ≤ 1) have been built which are very useful in tailoring many important parameters of LaTaON 2 . Band gap of LaTaON 2 becomes tunable by controlling the level of solid solutions with SrZrO 3 . Structural distortions, defects (e.g. Ta 4+ species) concentration and surface hydrophilicity of LaTaON 2 are largely improved by introducing SrZrO 3 in the structure. These modifications contribute to much enhanced photocatalytic activities of solid solutions for oxygen production which clearly outperform pristine LaTaON 2 under visible light illumination. Apparent quantum efficiency as high as 0.87% at 420 ± 20 nm was achieved at (LaTaON 2 ) 0.6 (SrZrO 3 ) 0.4 (x = 0.4). Further analysis suggest that introducing SrZrO 3 results in realignment of band edge positions of LaTaON 2 so as to be more appropriate for water splitting reactions.
研究领域:
材料科学
·
光催化化学
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产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2016
·
IF 7.354
Fangfang Wu,Gang Liu,Xiaoxiang Xu
LaTiO 2 N has been considered a promising candidate for efficient photocatalytic water splitting. However, its photocatalytic activity is often hampered by the presence of structural defects and poor charge mobility. In this work, we introduced Ca into the crystal structure of LaTiO 2 N via a simple co-precipitation method and investigated the photocatalytic and photoelectrochemical properties for the full range solid solution La 1− x Ca x TiO 2+ y N 1−y (0 ⩽ x , y ⩽ 1). Our results show that incorporating Ca into LaTiO 2 N induces a strong structural shrinkage as well as a space group change from I mma to P nma around a middle doping point ( x = 0.5). The presence of Ca effectively boosts the photocatalytic oxygen production and aids photocurrent extraction for LaTiO 2 N. The best photocatalytic activity was achieved for sample La 0.3 Ca 0.7 TiO 2.7 N 0.3 with oxygen production rate ∼66.96 μmol/h under visible light illumination ( λ ⩾ 420 nm), corresponding to apparent quantum efficiency ∼3.13%. XPS analysis revealed a substantial reduction in surface Ti 3+ species and a removal of A-site cation segregation for samples containing Ca. Further photoelectrochemical analysis highlights the critical role of Ca in enhancing the charge mobility of LaTiO 2 N. The better photocatalytic performance of Ca-modified LaTiO 2 N can be understood as a result of defect removal, high charge mobility, and improved surface charge migration pathways that considerably prolong the lifetimes of photogenerated charges.
研究领域:
材料科学
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化学工程
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能源科学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Xichen Sun,Pengfei Wang,Liuyan Tang,Ningning Li,Yan-Ru Lou,Yuezhou Zhang,Peng Li
An effective method capable of simultaneously providing antibacterial activity, blood glucose regulation, and angiogenesis promotion for healing bacteria-infected diabetic wounds is not reported to date, but urgently required. In this study, a hydrogel composite ( γ -PGA/PDA/GOx/WO x (PPGW)), endowed with these desired attributes is fabricated by incorporating polydopamine (PDA), glucose oxidase (GOx), and tungsten oxide (WO x ) nanowires into the poly( γ -glutamic acid) ( γ -PGA) framework. The exceptional photothermal conversion properties of PDA facilitated notable antibacterial effects on bacteria-infected diabetic wounds; GOx regulated high blood glucose by consuming glucose and generating hydrogen peroxide (H 2 O 2 ); while WO x nanowires displayed remarkable photocatalytic abilities, converting H 2 O 2 into oxygen (O 2 ) when exposed to 808-nm near-infrared radiation. Density functional theory calculations and experiments are conducted to confirm the mechanism of WO x -mediated photocatalytic degradation of H 2 O 2 to produce O 2 . These transformations aided in alleviating the hypoxic conditions in wounds associated with diabetes, expediting angiogenesis, and fostering cell crawling and proliferation. Consequently, the multifunctional hydrogel dressing PPGW, featuring photothermal, antibacterial, and enzyme-catalyzed activity reduces hyperglycemia at the wound site. Moreover, photocatalytic O 2 production represents a promising strategy for addressing chronic bacteria-infected diabetic wounds.
研究领域:
生物医学工程
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材料科学
·
糖尿病研究
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产品关联
DOI
高影响因子
RSC Advances
·
2020
·Vol. 10
·期 29
·17154-17162
·
IF 3.119
Ang Li,Yuxiang Liu,Xuejun Xu,Yuanyuan Zhang,Zhichun Si,Xiaodong Wu,Rui Ran,Duan Weng
Constructing Z-scheme heterojunctions is considered as an effective strategy to obtain catalysts of high efficiency in electron–hole separation in photocatalysis. Unfortunately, suitable heterojunctions are difficult to fabricate because the direct interaction between two semiconductors may lead to unpredictable negative effects such as electron scattering or electron trapping due to the existence of defects which causes the formation of new substances. Furthermore, the van der Waals contact between two semiconductors also results in bad electron diffusion. In this work, a MOF-derived carbon material as a Z-scheme photocatalyst was synthesized via one-step thermal treatment of MoS2 dots @Fe-MOF (MIL-101). Under visible light irradiation, the well-constructed Z-scheme (MoS2, γ-Fe2O3)/graphene photocatalyst shows 2-fold photocatalytic oxygen evolution activity (4400 μmol g−1 h−1) compared to that of γ-Fe2O3/graphene (2053 μmol g−1 h−1). Based on ultraviolet photoelectron spectrometry (UPS), Mott–Schottky plot, photocurrent and photoluminescence spectroscopy (PL) results, the photo-induced electrons from the conduction band of γ-Fe2O3 could transport quickly to the valence band of MoS2 via highly conductive graphene as an electron transport channel, which could significantly enhance the electron–hole separation efficiency as well as photocatalytic performance.
研究领域:
材料科学
·
光催化
✓ 已验证
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Zhuan Wang,Bo Yang,Xueying Zhao,Yushuai Chen,Dandi Wei,Lijuan Zhang,Xintai Su
Oxygen evolution reaction (OER) is the bottleneck of photocatalytic water splitting due to the slow four-electron transfer kinetics, and the construction of ultrathin materials is considered to be an effective means to solve the above problem. Herein, ultrathin γ-Fe 2 O 3 nanosheets (Fe 2 O 3 -NS) were prepared by a facile solution reduction-low temperature calcination method. The prepared photocatalyst has a leaf-like morphology with an average thickness of 2.0 nm and a large number of slit-like pores. Compared with γ-Fe 2 O 3 bulk, Fe 2 O 3 -NS exhibits excellent photocatalytic OER activity. The apparent quantum yield (AQE) and oxygen yield (measured at 420 nm) are 12.95% and 57.04%, respectively. The OER efficiency is superior to those reported iron oxide photocatalysts. This excellent performance may benefit from the ultrathin porous structure, appropriately narrow bandgap, and abundant oxygen vacancies . In addition, the photocatalyst shows good cycling stability, retaining 91.5% of the initial capacity in the fifth cycle test, which may be attributed to the magnetic cycling capability and good structural stability. This study confirms that Fe 2 O 3 -NS is a competitive candidate material for photocatalytic oxygen evolution and provides ideas for the design and construction of other defect-rich metal oxide nanosheets.
研究领域:
材料科学
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环境科学
·
能源科学
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DOI
高影响因子
GEOCHIMICA ET COSMOCHIMICA ACTA
·
2018
·
IF 4.69
Songhu Yuan,Xixiang Liu,Wenjuan Liao,Peng Zhang,Xiaoming Wang,Man Tong
Production of hydroxyl radicals ( OH) has been recently revealed upon oxygenation of sediments in redox-dynamic subsurface environments. In particular, Fe(II)-bearing clay minerals are the major sediment components contributing to OH production upon oxygenation, and the produced OH can oxidize contaminants and inactivate bacteria. Whereas, the mechanisms of OH production from oxygenation of Fe(II)-bearing clay minerals remain elusive. The objectives of this study were to identify the structural variation of Fe(II) entities during the oxidation of Fe(II)-bearing clay minerals by O 2 , and to unravel the mechanisms of electron transfer within the mineral structure and from mineral to O 2 for OH production. Nontronite (NAu-2, 23% Fe) which was chemically reduced to 54.5% Fe(II) in total Fe was used as a model Fe(II)-bearing clay mineral. Production of OH and oxidation of Fe(II) were measured during the oxidation of reduced NAu-2 by O 2 . A wide spectrum of spectroscopic techniques, including Fourier transform infrared spectroscopy (FTIR), Fe K-edge X-ray absorption spectroscopy (XAS), Mössbauer spectra, and X-ray photoelectron spectroscopy (XPS), were employed to explore the structural variation of Fe(II) entities in NAu-2 and the electron transfer within NAu-2 and from NAu-2 to O 2 . For 180 min oxidation of 1 g/L reduced NAu-2, a biphasic OH production was observed, being quick within the initial 15 min and slow afterwards. Production of OH correlates well with oxidation of Fe(II) in the reduced NAu-2. Within the initial 15 min, trioctahedral Fe(II)-Fe(II)-Fe(II) entities and edge Fe(II) in the reduced NAu-2 were preferentially and quickly oxidized, and electrons from the interior Fe(II)-Fe(II)-Fe(II) entities were most likely ejected from the basal siloxane plane to O 2 . Meanwhile, trioctahedral Fe(II)-Fe(II)-Fe(II) entities were mainly transformed to dioctahedral Fe(II)-Fe(II) entities. When the time of oxygenation was longer than 15 min, dioctahedral Al-Fe(II), Fe(II)-Fe(II) and Fe(II)-Fe(III) entities were slowly oxidized, and the interior electrons were transported through Fe(II)-O-Fe(III) linkages to edges and then ejected to O 2 . In the slow stage of oxidation, electrons from interior Fe(II) accumulated towards the near surface layers and fueled the regeneration of edge Fe(II) for OH production. In both stages, one-electron transfer mechanism with the involvement of O 2 − and H 2 O 2 applies for OH production from the oxidation of structural Fe(II) by O 2 . The mechanisms unraveled in this study advance the understanding of reactive oxygen species (ROS) production and structural Fe variation when Fe(II)-bearing clay minerals are oxygenated in redox-dynamic systems.
研究领域:
环境科学
·
矿物学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS LETTERS
·
2014
·
IF 2.269
Ming Yan,Yan Yan,Chao Wang,Wei Lu,Weidong Shi
In this letter, Ni 2+ doped InVO 4 nanocrystals were successfully synthesized by a simple one-pot microwave-assisted method. The energy bandgap of obtained samples can be precisely controlled by varying the Ni 2+ doping amount. The O 2 production rate of obtained Ni–InVO 4 nanocrystals is higher than that of pure InVO 4 nanocrystals under visible-light, which can be ascribed to the narrowed band gaps. The corresponding 1% doped sample N1 has the highest O 2 production rate (394 μmol/h) in all samples, which is 66% higher than the undoped sample N0.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Shumin Li,Jun Tan,Zhejun Jiang,Jin Wang,Zhengquan Li
Dye-sensitized systems show promising in photocatalysis because they can separate the tasks of light absorption, charge generation and surface catalysis to two coupled components. In this system, it is crucial to develop suitable catalysts capable of receiving dye-injected charges and having high activity to a given reaction. Aiming to photocatalytic H 2 and O 2 production, we present a metal-organic framework derived route to prepare bimetallic Fe-Ni-P nanotubes using Fe-Ni-MIL-88 nanorods as templates. When integrated with different dyes, these Fe-Ni-P nanotubes can serve as efficient catalysts for photocatalytic H 2 and O 2 production, respectively. Additionally, catalytic activities of such dye-sensitized systems can be conveniently regulated by tailoring the metal compositions in Fe-Ni-P nanotubes. The photocatalytic H 2 production of Fe 1 -Ni 2 -P can reach 5420 μmol g cat −1 h −1 under eosin-Y sensitization, which is 24 times and 6.7 times higher than Fe 2 P and Ni 2 P, respectively. The photocatalytic O 2 production of Fe 1 -Ni 2 -P can reach 900.3 μmol g cat −1 h −1 under [Ru(bpy) 3 ]Cl 2 sensitization, about 4.6 times and 2.9 times higher than Fe 2 P and Ni 2 P. The roles of different components in the system have been explored and corresponding working mechanism is proposed. This work demonstrates a new type of dye-sensitized systems consisting of bimetallic phosphides and provides a facile route to regulate their photocatalytic performance.
研究领域:
材料科学
·
光催化
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DOI
高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2018
·Vol. 20
·期 38
·24561-24569
·
IF 3.906
Ping Wang,Hengyan Yang,Ding Wang,AiYing Chen,Wei-Lin Dai,Xianglong Zhao,Junhe Yang,Xianying Wang
We report a feasible strategy via hydrothermal crystallization to activate Kagome lattice-structured Cu3V2O7(OH)2·2H2O volborthite mineral as a stable visible-light-driven photocatalyst. It was demonstrated to play a crucial role in stimulating absorption ability and photodegradation performance for the removal of methylene blue present in high concentration. In contrast, direct calcination was almost ineffective, whereas post-calcination was significantly detrimental. Moreover, the photocatalytic water oxidation activity of hydrothermally crystallizated volborthite was comparable to that of BiVO4, and it was clearly higher than those of WO3 and g-C3N4 from aqueous NaIO3 solution. By further in situ decoration with an optimum amount of CoOx cocatalysts (i.e., 2 wt%), the oxygen evolution rate of volborthite was greatly enhanced, and it was 1.6-fold, 1.8-fold and 2.9-fold higher than those of BiVO4, WO3 and g-C3N4, respectively. The importance of hydrothermal crystallization can be elucidated in terms of water-Kagome lattice structure interactions involving built-in intrinsic electric field and formation of single hydrogen bonds.
研究领域:
材料科学
·
光催化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）