Materials Today Energy
·
2025
·
IF 8.6
Binghong Wu,Xinru Wu,Dong-Hau Kuo,Xiao Tang,Xin Mao,Baoqian Yang,Zhengjie Su,Pengkun Zhang,Longyan Chen,Minhao Liu,Jinguo Lin,Xiaoyun Chen
To reveal the role of bi-vacancy defects and heterovalent states in oxysulfide catalysts for enhancing the photocatalytic hydrogen evolution reaction (PHER), we demonstrate a Br/W co-doped Zn(O,S) catalyst (labeled as Br/W-ZnOS) featuring abundant anionic oxygen vacancies (V O )/cationic zinc vacancies (V Zn ) bi-defects and heterovalent W 5+ /W 6+ states via a facile hydrolysis method. The co-doping of Br and W induces lattice distortions that enable neighboring atoms to leave the lattice, creating surfaces enriched with anionic V O and cationic V Zn defects. The synergistic effect between dual defects forms an efficient electron-hole separation system, enhancing the efficiency of electron-hole pair separation. Density functional theory calculation (DFT) demonstrates that the combination of Br/W co-doping and vacancies significantly reduces the water dissociation barrier and optimizes the surface ∗H generation rate of the photocatalyst. Thus, Br/W-ZnOS exhibits a PHER rate of 3415.7 μmol h −1 , which is 12.5 times higher than the undoped Zn(O,S) catalyst, and achieves an apparent quantum yield (AQY) of 15.41 % at 365 nm, while maintaining good stability with a PHER activity of 3288.1 μmol h −1 after five repeated cycles. This research provides a promising strategy for designing oxysulfide catalysts with synergistically engineered defects for efficient PHER.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Menglan Gao,Xiaobin Liao,Shuting Chen,Xiaoying Li,Yirou Zhang,Chao Chen,Huan Qi
Bromide ion (Br - ) in water sources has been found to affect the formation of carcinogenic non-brominated N-nitrosodimethylamine (NDMA) during ozonation of typical amines. The increasing bromide levels bring more concern due to climate change and industrial discharge, but its effects on actual water matrixes were still unclear. In this study, NDMA formation from three actual water matrixes during ozonation as the Br - concentration increased from 0 to 100 µM were investigated (promotion (100.4 ∼ 231.6 ng/L), promotion then inhibition (399.5 ∼ 461.2 ∼ 428.2 ng/L), and subtle influence (51.9 ± 6.9 ng/L)); from which the NDMA precursors were screened and 8 precursors were selected for exploring the influencing mechanisms. The results indicated that the roles of Br - on NDMA formation significantly depended on the water characteristics of actual matrixes. A total of 16 typical NDMA precursors, which were mainly derived from industrial, agricultural and pharmaceutical sources, were identified. Moreover, 6 brominated substance (Br-DMA, Br-UDMH, Br-DMSC, Br-DMS, Br-TMDS, Br 2 -TMDS), which were thought to play a crucial role in promoting NDMA formation, were also identified in actual water by precursor ion scan (PIS) method. Hypobromous acid (HOBr), which has been proved to be the culprit to the generation of brominated substances, tend to attack the electron-donating groups of amines, such as acylamino (–NHCO-R) or amidogen (–NH 2 ) groups. However, the reactive bromine species (∙Br and ∙Br 2 - ) was inclined to attack the aromatic and anti-oxidant moieties then result in Br - release, as no bromine substitution but free radical transfer reaction occurs. Therefore, decreasing HOBr formation is the crucial step to reduce NDMA generation. This work would provide technical guide for NDMA risks control during ozonation of Br - -amines co-containing water matrixes.
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CHEMISTRY OF MATERIALS
·
2025
·
IF 7
Wei Shen,Zhihua Chen,Junmin Xia,Jiayu Jiang,Yanfeng Chen,Yanxing He,Hao Cui,Wei Zhao,Suyun Liu,Shufen Chen
The soft ionic nature, tunable lattice structure, variable component, and solution processability make metal halide perovskite (MHP) materials good candidates as high-entropy materials. Although composition regulation of the X site can be easily achieved by mixing two types of halogens, it remains challenging to prepare high-entropy MHP (HEMHP) with three types of halogens due to the large octahedral factor (μ) difference of [PbX6]4–. Fundamental research is explored to synthesize HEMHP incorporating Cl–, Br–, and I– via μ regulation engineering, which breaks the limitation of a 6% Cl/I ratio in perovskite to achieve 116%. Doping AlCl3 in CsPbBrI2 could successfully reduce the μ differences for [Pb1–aAlaX6](4–a)–, shorten the Pb–X bond length, and enhance the Pb–X bond energy via the Al–X covalent bond. Therefore, the crystal distortion and halogen ion migration could be inhibited to form a homogeneous HEMHP, such as Cs1.18Pb0.92Al0.08(Cl0.13Br0.51I0.36)2.45L–0.81, Cs1.12Pb0.88Al0.12(Cl0.25Br0.49I0.26)2.53L–0.71, and Cs1.06Pb0.85Al0.15(Cl0.29Br0.46I0.25)2.43L–0.78. Such μ regulation engineering method is feasible and universal to use other metal ions (Zn2+, Mn2+, and In3+) to synthesize single-phase HEMHP. Furthermore, the optical band gap and emission peak wavelength for HEMHP and MHP are linearly dependent on their lattice distances, which is the intrinsic characteristic for composition-depended perovskite.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Hao Zhang,Hanxiao Zheng,Ying Wang,Runhua Yan,Dingyuan Luo,Wei Jiang
Petal bismuth salt semiconductors are promising as visible-light-driven photocatalysts, but their short service times due to strong oxidation limit their application. In this research, the in situ construction of a p–n heterojunction, by growing BiOX on a KBiO3 surface, is used as a strategy to improve the performance and stability. Evaluation of the photocatalytic degradation of crystal violet and phenol shows that the KBiO3/BiOX (X = Cl, Br, I) heterostructures exhibit significant improvement in photocatalytic performance and stability compared to KBiO3. The best one, KBiO3/(5.85%) BiOI, shows 98% degradation of crystal violet within 20 min, and of phenol within 1.5 h. No significant performance decay can be detected after repeated use. The development of KBiO3/BiOX heterostructure improves the applicability of KBiO3 as an efficient visible-light-driven photocatalyst.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Menglu Wang,Bolong Liang,Shumin Lin,Zhe Zhao,Hongbin He,Xiliang Li,Shu-xuan Liang
The magnetic Fe 3 O 4 @ZIF-8 with high adsorption properties and easy separation were embedded in BiOX (X = Cl, Br, I) to synthesize Fe 3 O 4 @ZIF-8@BiOX using a simple one-pot solvothermal strategy. The crystal structure, surface morphology, photoelectric properties, thermal stability and magnetic response of the three materials were compared and analyzed, and the effect on the removal of OTC and Cr(VI) from single and coexisting systems by adsorption-photocatalysis is discussed. The results show Fe 3 O 4 @ZIF-8@BiOI has the highest separation efficiency of photogenerated carriers upon photoexcitation and stronger light absorption capacity, and exhibits better adsorption-photocatalytic activity than the other two materials in the photocatalytic reduction of Cr(VI) (68 % and 65 % removal for single and coexisting systems) and degradation of OTC (86 % and 59 % removal for single and coexisting systems). It is noteworthy that in the coexistence of Cr(VI) and OTC, a slight decrease of removal occurred, which could be due to a competitive effect between two pollutants being greater than the synergistic effect. ∙O 2 - is the main active substances in the adsorption-photocatalysis process. Finally, this work demonstrates the excellent adsorption and photocatalytic ability of Fe 3 O 4 @ZIF-8@BiOI for the simultaneous removal of Cr(VI) and OTC, which has great potential for practical wastewater treatment.
研究领域:
环境科学
·
材料科学
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Linjie Wang,Xuechao Xu,Peng Liu,Mengzhu Wang,Xiangheng Niu,Jianming Pan
Abnormal levels of halide ions in drinking water have enormous threats to human health, and thus designing reliable and sensitive methods to quantify and distinguish these ions becomes extremely crucial. Herein, we develop a single-nanozyme colorimetric array based on target-induced differential surface passivation for the quantification and discrimination of Cl − , Br − and I − ions. Silver citrate (Ag 3 Cit) is designed as an oxidase mimic to efficiently catalyze the 3,3′,5,5′-tetramethylbenzidine (TMB) chromogenic reaction. When halide ions (Cl − , Br − and I − ) are present, due to their different precipitation interactions with the Ag(Ⅰ) entity in Ag 3 Cit, they can passivate the active surface of the nanozyme to various degrees, resulting in the inhibited TMB chromogenic reaction differentially. According to this principle, simple and efficient quantitative detection of Cl − , Br − and I − ions was achieved, with all the detection limits down to the nM level. By employing Ag 3 Cit as a single sensing element, a nanozyme catalysis-based colorimetric array was further established, and both individual and mixed ions were successfully distinguished by integrating the array with principal component analysis . Accurate identification of unknown samples was also verified via a double-blind protocol, indicating potential applications of the array in practice.
研究领域:
分析化学
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环境科学
·
生物医学工程
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PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2018
·
IF 3.849
Weirui Chen,Zulin Zhang,Xukai Li,Dan Wu,Ying Xue,Laisheng Li
Fe-Cu-MCM-41/O 3 was first used as an alternative to O 3 to control disinfection by-products generation from chlorinated-disinfection of Br-containing Diclofenac. Accompanying with decrease of TOC , THMs and HAAs had an initial increase, reaching the highest at 30 min, then gradually decreased. Coupling Fe-Cu-MCM-41 with O 3 successfully enhanced TOC removal and inhibited bromate, THMs and HAAs formation in post-chlorination when compared with those in ozonation . Four kinds of THMs and six kinds of HAAs were detected. CHCl 3 was main Cl-THMs and CHBrCl 2 was main Br-THMs. CHCl 2 COOH was the dominant Cl-HAAs and CHClBrCOOH was main Br-HAAs. A converse Br-THMs order was observed in O 3 and Fe-Cu-MCM-41/O 3 pre-treatment. Fe-Cu-MCM-41 decreased ozone exposure, reducing the direct reaction of O 3 with Br − to form bromate. More DBPs precursors in Fe-Cu-MCM-41/O 3 were removed by ·OH. H 2 O 2 , which generated during pre-treatment process, reduced HBrO/BrO − to Br − , inhibiting both its reaction with Br-DBPs precursors and bromate formation. The pre-treatment process changed intermediates’ properties and hydrophilic DOM was the dominant component. Hydrophobic acids and transphilic DOM were the main chlorine consuming intermediates and had major contribution to DBPs formation. Fulvic-like intermediates was suggested as precursors of Br-DBPs. Fe-Cu-MCM-41/O 3 were suggested as a good alternative to O 3 pretreatment.
研究领域:
环境科学
·
水处理工程
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高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Lei Zhou,Xin Wei,Junxiang Zhang,Xuecui Mei,Yun Li,Chaoyue Zheng,Furong Zhang,An Wen,Bin Wang
Sulfide solid electrolytes (SSEs) have some huge advantages in high room-temperature conductivity, good thermal stability, low interfacial resistance, etc. They are one of the ideal solid electrolytes for developing high energy density and high safety for all-solid-state lithium batteries (ASSLBs). However, the preparation of SSEs requires expensive Li2S as the raw material, whose high cost limits its practical application. Herein, a cost-effective SSE Li7.3P2.9S10.75X0.3 (X = F, Cl, Br, and I) was designed and prepared by using low-cost lithium and sulfur instead of expensive Li2S. Significantly, the cost of SSEs was reduced from $169.72 to $28.13 kg–1 based on replacing the Li2S strategy. Moreover, the prepared Li7.3P2.9S10.75X0.3 (X = F, Cl, Br, and I) solid electrolytes have a high ionic conductivity of 1.86–2.73 mS cm–1 at room temperature and a high voltage window of 5 V. On this basis, we assembled the all-solid-state lithium battery TiS2/Li7.3P2.9S10.75I0.3/Li–In, which presented a high initial discharge capacity of 219 mA h g–1 at room temperature and satisfactory cycle stability with a capacity retention of 86.7% after 100 cycles at 0.50 mA cm–2. This work provides an effective strategy for reducing the cost of SSEs, advancing the practical process of ASSLBs.
研究领域:
材料科学
·
能源技术
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高影响因子
Journal of Materials Chemistry C
·
2026
·
IF 5.1
Hai Ou,Xin An,Peng Li,Weikang Dong,Keke Guan,Jiaxin Qin,Yuanting Wu
CsPbX 3 (X = I, Br, Cl) perovskite quantum dots (QDs) have shown great potential in optoelectronic devices due to their wide tunable bandgap, high photoluminescence quantum yield, and narrow emission spectra. Currently, methods for regulating blue light emission through component engineering or dimensional engineering suffer from issues such as halogen phase separation and increased defects, making it difficult to meet the strict requirements of display technology for pure blue light (CIE y < 0.15). Additionally, traditional synthesis processes are complex and have poor compatibility with Micro-LED miniaturization technology, which restricts their industrial application. Therefore, this study proposes an efficient and green spray drying method. By dissolving the perovskite precursors and halide salts in an aqueous solution, CsPb(Cl/Br) 3 QDs can be rapidly (<10 s) synthesized without organic solvents, and continuous tuning from green to blue light is achieved. This method effectively suppresses surface defects and phase separation through Cl element encapsulation, significantly enhancing stability.Moreover, its excellent processability supports spraying and film formation on any substrate, enabling the direct preparation of highly uniform Mini/Micro-LED pixel units. This technology provides a new approach for large-scale, low-cost manufacturing of perovskite QDs and is expected to accelerate the commercialization process of next-generation display technologies.
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Small
·
2021
·Vol. 18
·期 8
·2106323
·
IF 13.281
Jingwei Zhu,Benlin He,Xinpeng Yao,Haiyan Chen,Yanyan Duan,Jialong Duan,Qunwei Tang
The precise phase control of Cs-Pb-Br derivatives from 3D CsPbBr 3 to 0D Cs 4 PbBr 6 highly determines the photovoltaic performance of all-inorganic CsPbBr 3 perovskite solar cells (PSCs). Herein, the preferred phase conversion from precursor to Cs-Pb-Br derivatives is revealed by theoretically calculating the Gibbs free energies (∆ G ) of various phase conversion processes, allowing for a simplified multi-step solution-processable spin-coating method to hinder the formation of detrimental 0D Cs 4 PbBr 6 phase and enhance the photovoltaic performance of a PSC because of its large exciton binding energy, which is regarded as a recombination center. By further accelerating the interfacial charge extraction with a novel 2D transition metal dichalcogenide ReSe 2 , the hole-free CsPbBr 3 PSC achieves a champion efficiency of 10.67% with an impressive open-circuit voltage of 1.622 V and an excellent long-term stability. This work provides an in-depth understanding on the precise Cs-Pb-Br perovskite phase control and the effect of derivatives on photovoltaic performance of advanced CsPbBr 3 PSCs.
研究领域:
材料科学
·
光伏技术
·
纳米材料
·
能源化学
·
半导体物理
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高影响因子
POLYMER
·
2023
·
IF 4.6
Xinlin Zhu,Jiacheng Yi,Wenjie Wang,Siyu Qu,Qinghua Deng,Jingyu Wu,Yang Zhou,Wuwei Yan,Yong Yang
The all-solid-state polymer electrolyte (SPE) with superior electrochemical performance and stability is the most significant part for the development of high safety and reliable batteries . In this work, the ether linkage and imidazolium ionic liquid are incorporated into the modified macromolecular cellulose network via atom transfer radical polymerization for the construction of brush-like cellulose bromide-poly(ethylene glycol) methyl ether methacrylate@1-vinylimidazole ionic liquid (CB-PEGMA@IL) and cellulose bromide-1-vinylimidazole ionic liquid@poly(ethylene glycol) methyl ether methacrylate (CB-IL@PEGMA) composite polymers . The crystallinity of pristine CB is largely decreased on account of the synergistic effect of ionic liquids and ether linkage. In particular, CB-PEGMA@IL presents a lower crystallinity and superior electrochemical performances than that of the CB-IL@PEGMA. With a wide electrochemical stability window (5.3 V vs Li/Li + ), the CB-PEGMA@IL based SPE presents a high ionic conductivity (1.2 × 10 −4 S cm −1 ) and record Li + transference number (0.32). LiFePO 4 /Li battery assembled with CB-PEGMA@IL-SPE shows excellent cycling performance (beyond 150 cycles at 0.2 C) and good rate capacity. Moreover, the overpotential of CB-PEGMA@IL-SPE based symmetric battery can keep ∼0.03 V even after 200 h cycling (100 μA cm −2 ). The soft-packed battery based on CB-PEGMA@IL-SPE can withstand bending and present stable voltage output upon folding at various angles. This rigid-flexible hybrid SPE provides a unique candidate for the fabrication of wearable high-tech electronic devices.
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Materials Today Physics
·
2022
·
IF 11.021
Siqi Sun,Pei Jia,Qizhang Huang,Min Lu,Po Lu,Feisong Qin,Guang Sun,Yanbo Gao,Xue Bai,Zhennan Wu,Yu Zhang
Despite rapid development of perovskite nanocrystal (PeNC) light-emitting diodes (LEDs), it remains challenging to achieve efficient and stable blue PeLEDs , especially for pure-blue PeLEDs required for displays. Mixed halide CsPb(Br/Cl) 3 NC is a common strategy to achieve pure-blue emission, but suffers from low photoluminescence quantum yield (PLQY) and spectra instability. Here, a facile approach for the synthesis of high-quality pure-blue emitting CsPb(Br/Cl) 3 NCs is reported by introducing an organic sulfonate, phenyl trifluoromethanesulfonate (PTFMS), which works as an efficient surface passivator. As a result, the optimized PeNCs achieve a high PLQY of 85% and enhanced conductivity. Furthermore, the LED based on the optimized PeNCs is developed with pure-blue emission at 469 nm, which yields an external quantum efficiency (EQE) of 1.20% and luminance of 355 cd m −2 . More impressively, the device shows excellent spectra and operation stability under voltage bias , resulting from the suppressed ion migration channels by efficient defect passivation .
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