Molecular Catalysis
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2023
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IF 4.6
Lianyang Zhang,Yue Meng,Bo Xie,Zheming Ni,Shengjie Xia
The activity of single-crystal catalysts with different crystal faces varies greatly, and the construction of catalysts with highly exposed active facets is essential for the improvement of photocatalytic performance. In this paper, Cu 2 O (100) crystal facets were transformed into high degrade-active Cu 2 O (111) crystal facets by doping with halogen atoms Br for the photocatalytic degradation of tetracycline. The effect of the optimal Br/Cu 2 O ratio on the degradation activity was investigated by adjusting the amount of Br. Meanwhile, based on photocatalytic degradation performance tests, photoelectric performance characterization and theoretical calculations, it was found that the doped Br-Cu 2 O introduced impurity energy levels, reduced the band gap, broadened the absorption range of the photocatalyst under visible light, and enhanced the oxidation capacity and the rate of photogenerated electron leap. In addition, the highly active Cu 2 O (111) crystal surface facilitates the adsorption of oxygen to generate superoxide radicals and promote the photocatalytic reaction. The synergistic effect of these two aspects promotes the efficient degradation of tetracycline by Br-Cu 2 O. This work provides a promising idea for the design and construction of highly efficient active surface highly exposed photocatalysts.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Guoan Wang,Tingting Huo,Quanhua Deng,Fei Yu,Yuguo Xia,Haiping Li,Wanguo Hou
The oxygen vacancy (Ov) in photocatalysts plays a significant role for N 2 fixation, but effective and simple means for creation of Ov are in urgent demand. Herein, surface-layer Br doping was confirmed to create massive surface Ov in Bi 2 MoO 6 in a solvothermal process, with the product (BMO-Br-Ov) exhibiting remarkably enhanced N 2 chemisorption and activation, photoinduced charge separation, and thus photocatalytic N 2 fixation, compared with bulk Bi 2 MoO 6 , with an apparent quantum yield at 420 nm reaching 0.52% in pure water and 2.56% in the methanol aqueous solution. The charge separation enhancement benefits from the Ov introduced defect level and Br doping and surface Ov modification induced band-level difference between the surface and the inside in BMO-Br-Ov that leads to fabrication of the surface/inside homojunction. This work provides a simple way to create surface Ov in Bi 2 MoO 6 and may direct Ov creation in other Bi-based photocatalysts for efficient N 2 fixation.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Yueli Liu,Qitao Li,Wenchao Zhang,Zifan Yang,Sijie Zhao,Wen Chen
All-inorganic CsPbI3 perovskite quantum dots (QDs) have attracted great attention since emerging as a new class of materials with superior light-harvesting properties and enhanced thermal stability compared to organic–inorganic hybrid perovskites. However, poor phase stability remains a bottleneck for practical applications. In the present work, CsPb(I1–xBrx)3 perovskite QDs are synthesized by Br doping to increase the tolerance factor for the improvement of phase stability, and the balance between the stability of solar cells and the power conversion efficiency (PCE) is considered by adjusting the Br doping content. It is found that the phase stability of CsPb(I1–xBrx)3 QDs is much improved, while their band gap increases from 1.77 to 1.89 eV when the Br doping content increases from 0 to 30%. CsPbI2.4Br0.6 QD-based perovskite solar cells (PSCs) achieve a proper balance between high PCE and stability; the PCE is 12.31%, approaching that of the CsPbI3-based PSCs (14.13%), and may retain 87% of the initial efficiency after 15 days of storage in ambient air.
研究领域:
材料科学
·
光伏技术
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
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IF 14.229
Xin Hu,Huiping Zhao,Ying Liang,Rong Chen
Solar-driven molecular oxygen activation is of great importance for reactive oxygen species (ROS) production in environmental remediation. In this work, a convenient bromine doping strategy was developed to mediate the energy level of Bi 2 O 2 CO 3 for molecular oxygen activation. The band structure and DFT calculation demonstrate that the Fermi level of Bi 2 O 2 CO 3 elevates after bromine doping, which promotes the molecular oxygen activation and ROS production. The Br-doped Bi 2 O 2 CO 3 exhibits remarkably enhanced photocatalytic ability and could degrade 95% of the ciprofloxacin within 30 min. Moreover, HPLC-MS analysis elucidates that the pyrrolidone ring degradation process is the dominate pathway in ciprofloxacin degradation over Br-doped Bi 2 O 2 CO 3 , resulting in the decrease of antimicrobial activity of the degradation products and the risk of drug-resistance. This work not only provides a molecular oxygen activation strategy via energy level mediation, but also helps us to further understand the relationship between the elemental doping and molecular oxygen activation.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Mingrui Guo,Meng Chen,Jixiang Xu,Chao Wang,Lei Wang
Introducing defects and heteroatoms on carbon nitride (g-C 3 N 4 , CN) framework are effective ways to enhance its photocatalytic activity by regulating light absorption and charge carriers separation. Herein, a mechanochemical method was employed to synthesize Br-doped C, N-deficient CN (CN V -mCN-Br) via ball-milling of N-containing precursor and 6-Bromopyridine-3-carbaldehyde (BrPyCHO) followed by calcining. The ball-milling-evolved mechanical forces and BrPyCHO-derived HBr induced formation of C, N vacancies and C-Br bond in CN V -mCN-Br framework. The CN V -mCN-Br exhibited curled nanosheets morphology and separated electrons-holes distribution. The photocatalytic H 2 evolution rates of 1 %Pt-loaded CN V -mCN-Br in distilled water and simulated seawater were 22.21 and 34.41 mmol g –1 h −1 , respectively with 10% triethanolamine . The corresponding apparent quantum yields were 25.87% and 40.08% at 420 nm. This work provides a facile technique to simultaneously introduce defect and heteroatom in CN for high-efficiency photocatalytic H 2 evolution.
研究领域:
材料科学
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能源化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Tianyi Xu,Dongxu Jiao,Lei Zhang,Haiyan Zhang,Lirong Zheng,David J. Singh,Jingxiang Zhao,Weitao Zheng,Xiaoqiang Cui
Development of efficient electrocatalysts requires construction of catalytic surfaces with moderate H adsorption energy. Here, we address this challenge by Br-induced formation of P-poor defective nickel phosphide and show that the H adsorption energy can be optimized by regulating the vacancy concentration. We show that when such defective Ni 12 P 5−x Br x nanoparticles are distributed on the surface of Ni 2 P nanosheets (Ni 12 P 5−x Br x /Ni 2 P NS), excellent catalytic activity for water splitting is obtained in alkaline media. Density functional theory computations revealed that Br doping induce the formation of a P-poor nickel phosphide with vacancies, leading to an optimal H adsorption strength with a volcano-type relationship. This is the best reported for a non-precious metal phosphide at present: the overpotential for HER is 18 mV at 10 mA cm −2 and 155 mV for OER. This leads to an exceptionally low cell voltage requirement of only 1.44 V to drive overall water splitting in an alkaline electrolyzer.
研究领域:
材料科学
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电化学
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DOI
高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 14
·2423
·
IF 5.719
Qian Zhang,Wuyang Nie,Tian Hou,Hao Shen,Qiang Li,Chongshang Guan,Libing Duan,Xiaoru Zhao
Crystal facet engineering and nonmetal doping are regarded as effective strategies for improving the separation of charge carriers and photocatalytic activity of semiconductor photocatalysts. In this paper, we developed a facial method for fabricating oxygen-deficient Br-doped BiOCl nanosheets with dominating {001} facets through a traditional hydrothermal reaction and explored the impact of the Br doping and specific facets on carrier separation and photocatalytic performance. The morphologies, structures, and optical and photocatalytic properties of the obtained products were characterized systematically. The BiOCl samples prepared by the hydrothermal reaction exhibited square-like shapes with dominating {001} facets. Photodeposition results indicated that photoinduced electrons preferred to transfer to {001} facets because of the strong internal static electric fields in BiOCl nanosheets with dominating {001} facets. Br doping not only contributed to the formation of impurity energy levels that could promote light absorption but introduced a large number of surface oxygen vacancies (VO) in BiOCl photocatalysts, which was beneficial for photocatalytic performance. Moreover, the photocatalytic activities of these products under visible light were tested by degradation of rhodamine B (RhB). Because of the synergistic effect of the dominating {001} facets, Br doping, and rich VO, oxygen-deficient Br-doped BiOCl nanosheets exhibited improved carrier separation, visible light absorption, and photocatalytic efficiency.Keywords:BiOCl nanosheets;Br doping;surface facet;oxygen vacancies;photocatalytic performance
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Jiayu Gu,Mingzhou Wu,Linlin Wang,Fengling Liu,Suhao He,Minrui Ding,Yuye Yao,Neng Tao,Haitao Sha,Zhaobing Guo,Huimin Zhou,Pin Zhou,Pengxiang Qiu
Photocatalyst modification by energy level engineering is crucial for efficient free radical generation. Here, a novel strategy was employed to construct bromine-doped Bi 2 MoO 6 (BMO-Br) followed by an in-situ approach using Cetyltrimethylammonium bromide (CTAB) as the bromine (Br) precursor. The Br doping effectively modulated the energy band, increasing the oxygen vacancy concentration in Bi 2 MoO 6 . The modification significantly enhanced photoinduced charge separation and active free radical generation, leading to superior photocatalytic performance. The photocatalytic bacteriostatic and sulfamethazine (SM) degradation efficiency over BMO-Br-4 reached 100% and 70% within 60 min and 150 min, respectively. This work highlighted a facile yet effective strategy for tailoring the photocatalyst properties, demonstrating promising potential for various photocatalytic applications.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Jun Wang,Changqing Yang,Mingli Fu,Daiqi Ye,Lan Fan,Yun Hu
Different Br-doped metal-organic frameworks (MOFs) derived (Br x @UiO-66) have been prepared by heat treatment using UiO-66 as the precursor. The experimental results showed that Br 0.2 @UiO-66 exhibited the best photocatalytic oxidation and adsorption performances toward acetaldehyde. In the dynamic system, the acetaldehyde removal rate and adsorption capacity of Br 0.2 @UiO-66 were 93.2 % and 230.59 mg/g, respectively. The improvement of the photocatalytic performance can be attributed to the presence of Br ions and C Br bonds, which facilitated the rapid separation of electrons and holes and the production of •O 2 − . In addition, Br 0.2 @UiO-66 had a better adsorption performance than 300UiO-66, mainly because of the increased Lewis acidity of the metal active sites due to Br doping. Radical capture experiments indicated that •O 2 − and e - were the primary active substances in acetaldehyde oxidation , and allowed establishing the possible mechanism of acetaldehyde oxidation. This work shows that MOFs can have high catalytic oxidation performances toward volatile organic compounds (VOCs) while retaining their adsorption capacity, and can be used for practical applications in the adsorption-catalytic integrated degradation of VOCs.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry C
·
2020
·Vol. 9
·期 6
·2016-2023
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IF 7.059
Fengyou Qin,Hongjun Tian,Minxing Yan,Yanjun Fang,Deren Yang
Perovskite light-emitting diodes (PeLEDs) have drawn tremendous research attention recently. However, they are mainly prepared via solution processes, while the devices fabricated using the all-vacuum deposition procedure still remain largely unexplored. In this work, we prepared a cesium-lead-bromide perovskite film using the vacuum deposition method, and realized a more balanced stoichiometry by replacing some CsBr with NaBr. It was discovered that the introduction of an appropriate amount of NaBr not only reduced the insulating Cs4PbBr6 phase in the active layer, but also passivated the trap states effectively, which resulted in a 2-fold increase of the peak external quantum efficiency (EQE) of the PeLEDs to 2% with the maximum luminance reaching close to 40 000 cd m−2 and significantly improved device operational stability compared to the undoped counterparts. Furthermore, we fabricated the first top-emissive silicon-based PeLED using the all-vacuum deposition method based on the NaBr doped perovskite films, and achieved a peak EQE of 0.33%, which has provided a promising alternative way for the design and preparation of high-performance silicon-based display devices in the future.
研究领域:
材料科学
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光电技术
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半导体物理
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Meihan Liu,Haoran Fu,Sijie Yang,Hongyang Zhao,Zhibin Ma,Qiuming Fu,Hong Tao,Shu-Hua Yao,Yibo Han,Weidong Man,Zhenxiang Cheng
Two-dimensional (2D) hybrid perovskites have been garnering increasing attention across various fields due to their rich optical, electrical, optoelectronic, and magnetic properties. Current growth techniques only offer millimeter-scale or polycrystalline perovskites, which present a major barrier to the practical large-scale applications of these materials. In this study, we successfully prepared a series of BA2CuCl4–xBrx perovskite single-crystalline nanosheets with centimeter size using a controlled cooling growth method. Characterization results suggest that the obtained single-crystalline nanosheets are of high quality and that Br is uniformly doped. Moreover, these single-crystalline nanosheets exhibit ferromagnetic ordering at low temperatures, with the Curie–Weiss temperature increasing from 14.2 to 16.5 K as Br-doping concentration increases. Our approach provides a potential solution for the scalable synthesis and application of hybrid perovskites. At the same time, this family of 2D magnetic perovskites with tunable optical properties holds great potential for future spintronics applications.
研究领域:
材料科学
·
自旋电子学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiaoxiao Wang,Awei Guo,Yunlong Wang,Zhipeng Chen,Yuxuan Guo,Haijiao Xie,Weilong Shan,Junjie Zhang
Electrochemical conversion of CO 2 into chemical feedstock , such as an energy-dense liquid product (formate), is desirable to address the excessive emission of greenhouse gases and store energy. Cu-based catalysts exhibit great advantages in electrochemical CO 2 reduction reaction (eCO 2 RR) due to their low cost and high abundance, but suffer from low selectivity of formate. In this work, a facile one-pot approach is developed to synthesize CuBr nanoparticle (CuBr NP) that can conduct in situ dynamic restructuring during eCO 2 RR to generate Br-doped Cu NP. The in situ-formed Br-doped Cu NP can afford up to 91.6% Faradaic efficiency (FE) for formate production with a partial current density of 15.1 mA·cm −2 at −0.94 V vs. reversible hydrogen electrode (RHE) in an H-type cell. Moreover, Br-doped Cu NP can deliver excellent long-term stability for up to 25 h. The first-principles density functional theory (DFT) calculations show that the doped Br can regulate the electronic structure of Cu active sites to optimize the adsorption of the HCOO* intermediate, greatly hindering the formation of CO and H 2 . This work provides a strategy for electronic modulation of metal active site and suggests new opportunities in high selectivity for electrocatalytic reduction of CO 2 to formate over Cu-based catalysts.
研究领域:
材料科学
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环境科学
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电催化
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产品关联
DOI
PubMed
高影响因子
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