ACS Catalysis
·
2025
·
IF 13.1
Zhiqiang Qiu,Zhong-Pan Hu,Junyu Liu,Jingfeng Han,Shiyu Xia,Min Li,Yang Zhao,Jingrun Chen,Svetlana Mintova,Yingxu Wei,Zhongmin Liu
Conventional supported metal catalysts in propane dehydrogenation (PDH) face critical challenges due to sintering-induced deactivation at high reaction temperatures. Herein, we develop a series of highly stable atomically dispersed metal-Beta catalysts by embedding single metal atoms (such as V, Cr, Fe, Zn, and Ga) into the dealuminated H-Beta zeolite framework. Unlike the pristine H-Beta zeolite with Brønsted acid sites, the embedded metals possess a distorted tetrahedral structure and typical Lewis acidic properties, which exhibit good C–H bond activation rather than C–C bond activation observed on Brønsted acid sites. Among these metal-Beta zeolites, the Cr-Beta zeolite with an ultralow density of ∼128 framework atoms per Cr atom exhibits notable performance in PDH. Through HAADF-STEM, X-ray absorption spectroscopy (XAS), and isotope labeling FTIR, the local coordination environment of framework-embedded Cr species is unambiguously identified as a distorted tetrahedral geometry {(≡SiO)3Cr···(HO–Si≡)} with three Cr–O–Si bonds and one Cr···OH–Si linkage. Kinetic investigations and deuterium-labeling results demonstrate that propane activation occurs on isolated Cr Lewis sites with adjacent O atoms that facilitate the reception and release of hydrogen species. These findings provide valuable strategies for the rational design of supported metal catalysts for alkane activation and offer great insights into recognizing the local coordination structures of heteroatoms in zeolites.
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Journal of Central South University
·
2022
·Vol. 29
·期 5
·1447-1462
·
IF 2.392
Yang Ting,Hu Xin-yu,Wang Jun-tao,Yang Tian-li,Wang Wen-lei
A series of In x Sb 2− x S 3 nanosheets modified g-C 3 N 4 (In x Sb 2− x S 3 -TCN) heterojunctions with different g-C 3 N 4 contents were fabricated by an in situ deposition method. All the In x Sb 2− x S 3 -TCN composites were applied as photocatalysts in Cr(VI) polluted water treatment and the results displayed that In x Sb 2− x S 3 -TCN could effectively remove Cr(VI) under visible light through synergistic effects of adsorption and photocatalytic reduction. Especially, In x Sb 2− x S 3 -TCN-70 (70 mg g-C 3 N 4 ) exhibited the most excellent adsorption and photocatalytic reduction performance among all composites, which possessed a high equilibrium adsorption capacity of 12.45 mg/g in a 30.0 mg/L Cr(VI) aqueous solution, and reduced Cr(VI) to Cr(III) within 10 min under visible light irradiation. DRS and PL results indicated that the interfacial coupling effect between g-C 3 N 4 and In x Sb 2− x S 3 enhanced the utilization efficiency of visible light and suppressed photoinduced carrier recombination, which improved the photocatalytic activity of composites. Moreover, the photocatalyst exhibited satisfactory reduction activity and good stability after 5 cycles of Cr(VI) adsorption-photoreduction.
研究领域:
材料科学
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环境科学
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RSC Advances
·
2025
·Vol. 15
·期 18
·14227-14234
·
IF 4.6
Yingying Shen,Huan Cao,Miaomiao Du,Xinfeng Wang,Jia Qin
This study examines the adaptability of carbonate mineralizing bacteria in Cr(III)-contaminated environments with varying Cr(III) concentrations and their response mechanism via EPS. Cr(III) removal efficiency declined with concentrations exceeding 1000 mg L−1, while the removal amount continued to rise, indicating strong Cr(III) tolerance in the bacterium. Analysis of dynamic changes in EPS revealed a significant increase in production, with polysaccharides and proteins playing key roles in Cr(III) binding. A notable increase in mannose in the monosaccharide composition of EPS suggests its involvement in Cr(III) binding. Moreover, alterations in the protein secondary structure, such as a reduction in α-helix content and an increase in β-sheet and random coil structures, may enhance EPS interaction with Cr(III). These findings demonstrate that EPS contributes to heavy metal remediation not only through its polysaccharide components but also through changes in protein structure, offering a new theoretical foundation for Cr(III) bioremediation.
研究领域:
环境科学
·
微生物学
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PubMed
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2023
·Vol. 87
·期 9
·2061-2078
·
IF 2.7
Su Ya,Kang Yumeng,Huang Qinya,Zhang Jiahao,Liu Jinhua,Hu Zhaoyong,Liu Zhanchao,Liu Yan
View large Download slide View large Download slide Close modal The novel Cr(VI) anion-imprinted polymer (Cr(VI)-IIP) was prepared by a surface imprinting technique with bifunctional monomers pre-assembly system based on mesoporous silicon (SBA-15). The synthesized Cr(VI)-IIP was characterized by Fourier transmission infrared spectra (FT-IR), energy dispersive spectrometer (EDS), scanning electron microscope (SEM), transmission electron microscope (TEM), X-ray powder diffractometer, N 2 adsorption–desorption and thermogravimetric analysis (TGA), proving to be with a highly ordered mesoporous structure, as well as favorable thermal stability. The saturated adsorption amount was 96.32 mg/g, which was 2.7 times higher than that of non-imprinted polymer (NIP). Kinetic experiments showed that the adsorption equilibrium state was obtained within 70 min. In addition, in the selectivity experiments, Cr(VI)-IIP exhibited strong specific recognition ability for Cr(VI) and could realize the separation of Cr(VI) and Cr(III) from an aqueous solution. The dynamic adsorption experiments exhibited that the dynamic adsorption efficiency of Cr(VI)-IIP was as high as 71.57%. Meanwhile, the dynamic regeneration experiments showed that the adsorption amount of Cr(VI)-IIP did not decrease significantly after repeating for five times. All of the findings suggested that Cr(VI)-IIP could achieve precise identification as well as efficient separation of Cr(VI) from aqueous solution. Preparation of Cr(VI) anion-imprinted polymer (Cr(VI)-IIP) by bifunctional monomers pre-assembly system. The Cr(VI) imprinted sites formed by the coordination of bifunctional monomers and template ions could realize the separation of Cr(VI) and Cr(III). Cr(VI)-IIP exhibited superior selectivity compared to other common adsorbents and Cr(VI) imprinted polymers prepared by a single functional monomer.
研究领域:
环境科学
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高分子化学
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吸附技术
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材料科学
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水处理
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高影响因子
JOURNAL OF SUPERCRITICAL FLUIDS
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2022
·
IF 4.514
Jianqiao Yang,Shuzhong Wang,Jiahuan Wang,Jinlong Wang,Baoquan Zhang,Lu Liu,Wei Liu,Yanhui Li,Donghai Xu
In this study, the erosion-corrosion experiment of Ni based alloys in high-temperature and high-pressure supercritical water environment was performed. SiO 2 and Al 2 O 3 particles with the average diameter of 30 µm and 50 µm were used as erodent. The special designed specimens were fixed on a blade impeller , and the erosion tests were performed in a high pressure autoclave with a magnetic stirrer system. Results show that the basic corrosion mechanism is not changed by the erosion process. A Cr-rich inner oxide layer and a Fe/Ni rich outer oxide layer were formed on the alloy surface. However, the oxidation rates of the alloys were affected by the erosion process. Parts of the outer Fe and Ni oxides were removed by the erodent particles during the tests. The inner Cr oxide layer still exists owing to the self-healing ability of the Cr 2 O 3 layer, acting as a barrier to resist further corrosion of the alloys. The factors that affect the degree of erosion and the erosion-corrosion mechanism in SCW environment is analyzed.
研究领域:
材料科学
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腐蚀科学
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高温高压环境材料行为
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表面工程
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能源材料
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高影响因子
CRYSTENGCOMM
·
2020
·Vol. 23
·期 2
·482-491
·
IF 3.117
Lin-Hui Wu,Shu-Li Yao,Jing Li,Hui Xu,Teng-Fei Zheng,Sui-Jun Liu,Jing-Lin Chen,He-Rui Wen
A novel luminescent CdII-based metal–organic framework {[Cd(BBIP)(TBIP)]·EtOH}n (1) derived from the multidentate 5-tert-butylisophthalic acid (H2TBIP) and the semi-rigid N-donor 3,5-bis(benzimidazol-1-yl)pyridine (BBIP) has been solvothermally synthesized and structurally characterized by using infrared spectroscopy, thermal analysis, single-crystal X-ray diffraction and powder X-ray diffraction. The adjacent CdII ions are linked by two carboxylate groups of one TBIP2− ligand with chelating mode to form a one-dimensional CdII-TBIP2− chain, which is further connected by the BBIP ligand to obtain a two-dimensional network. Interestingly, the fluorescence experiments indicate that 1 could be considered as a good multi-responsive sensing material for detecting Fe3+, MnO4−, Cr2O72−, salicylaldehyde (SA) and ethylenediamine (EDA) via the turn-off effect, with the detection limits of 0.53, 0.98, 3.6, 0.42 and 5.3 ppm, respectively. The luminescence quenching effect induced by Fe3+ could be mainly ascribed to the competitive absorption mechanism. The electron-transfer transition and competitive absorption mechanism could be used to explain the luminescence quenching of MnO4− and Cr2O72−. The turn-off effect of 1 on SA could be ascribed to the photoinduced electron-transfer and competitive absorption mechanisms. Meanwhile, the possible mechanism of fluorescence quenching caused by EDA could be attributed to the structure collapse. More importantly, 1 could be regenerated and reused after five cycles for Fe3+, MnO4−, Cr2O72− and SA detection. In a nutshell, 1 could be employed as a multi-responsive luminescent sensor used for the highly selective and sensitive detection of metal ions, anions and small organic molecules.
研究领域:
材料科学
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分析化学
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高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2022
·
IF 3.475
Yuchao Zhu,Qiang Wei,Qinyu He,Deyang Chen,Than Zaw Oo,Su Htike Aung,Fuming Chen
Capacitive deionisation (CDI), as a novel electrochemical technology, has attracted a fast-growing research interest over the past years. However, the single function of salt removal limits further development of conventional CDI systems. Herein, we propose a multi-function CDI device, which can achieve the electrochemical desalination, degradation of organic pollutants and removal of heavy metal ions through the redox electrocatalytic deionisation technology. Sulphur-doped reduced graphene oxide (S@rGO) is utilised as the anode to catalyse the degradation of rhodamine B. The Pt-coated graphite paper is used as a cathode for the removal of dichromate ions by the electro-reduction process. The voltage plateau of S@rGO is reduced by ∼0.35 V compared with the pure carbon cloth electrode, indicating the effectiveness of S@rGO as the catalyser. The salt feed is desalted to ∼0.74 mS·cm−1 level at a current density of 1 mA·cm−2. The degradation efficiency of rhodamine B (RhB) and potassium dichromate are 99.1% and 55.3%, respectively. The effects of different current densities and cycling are also investigated. This work is significant for the multi-functional process of water treatment and the device design.Synopsis : The single function of salt removal limits the further development of the CDI system. A multi-function CDI device is proposed to achieve electrochemical desalination, organics degradation and dichromate ion removal.
研究领域:
环境科学
·
材料科学
·
电化学工程
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Pei Yu,Yulong Xiang,Xiaoli Dong,Yu Wang,Jialin Niu
The development of heterojunction photocatalysis provides an efficient, cost-effective, and environmentally sustainable approach to mitigating heavy metal contamination in the ecosystem. In this work, ZnIn 2 S 4 /H 2 Ti 3 O 7 heterojunctions have been successfully constructed via the in-situ growth of ZnIn 2 S 4 on H 2 Ti 3 O 7 nanowires. This rational structure enhances the separation efficiency of photogenerated carriers and suppresses carriers recombination. The ZnIn 2 S 4 /H 2 Ti 3 O 7 heterojunction exhibits significantly enhanced performance in the photoreduction of Cr(VI), and under 8 min illumination, it can achieve 100% photoreduction efficiency. The active species capture experiment confirmed that electrons served as the primary active species in the photocatalytic reduction of Cr(VI). This work offers support for the rational design of highly efficient heterojunction photocatalyst dedicated to environmental remediation.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Xufa Peng,Yiyi Yangliu,Bilong Liu,Zhuangzhi Wu,Hao Fei,Dezhi Wang
The electrochemical nitrogen reduction reaction (NRR) offers a sustainable route for ammonia production under ambient conditions, but its efficiency remains limited by sluggish N2 activation and competition from the hydrogen evolution reaction (HER). Rhenium disulfide (ReS2), characterized by weak interlayer coupling and an anisotropic electronic structure, provides a promising platform for nitrogen electrocatalysis; however, the limited abundance and insufficient reactivity of its intrinsic active sites restrict its NRR performance. Here, we introduce a Cr-Vs (sulfur vacancy) pair engineering strategy that transforms the local coordination environment of ReS2 into an electronically differentiated active site. Cr incorporation thermodynamically facilitates the Vs formation, generating a reconstructed Cr-Vs configurations with substantially modified local electronic states. This reconstruction optimizes Re 5d-N 2p orbital hybridization, thereby selectively stabilizing key hydrogenated nitrogen intermediates. Meanwhile, the Cr-Vs pair selectively tunes the competition between NRR and HER, preferentially enhancing the intrinsic NRR activity. Consequently, the optimized RSC-5 catalyst delivers an NH3 yield rate of 67.70 ± 0.72 μg mg-1cat. h-1 and a Faraday efficiency of 10.53 ± 0.38%. This work establishes dopant-vacancy coupling as a generalizable strategy for reconstructing local coordination and decoupling competing reaction pathways, offering design principles for developing selective electrocatalysts for sustainable ammonia synthesis.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Yinze Yang,Yan Du,Wen Yang,Yueru Yan,Yipeng Wang,Rujin Zhang,Huishan Shang,Lili Zhang,Yafei Zhao,Bing Zhang
Reasonable design core@shell heterostructures is essential for efficient photocatalytic reduction of Cr(VI) in water, as such architectures not only enhance light absorption but also facilitate light-induced charge separation and transfer. Herein, ZnIn 2 S 4 (ZIS) nanosheets were grown in situ on NiCo 2 O 4 hollow nanospheres to construct a NiCo 2 O 4 @ZIS heterostructured photocatalyst for efficient Cr(VI) reduction. The optimal 6 wt% NiCo 2 O 4 @ZIS achieves 100 % photocatalytic reduction efficiency for Cr(VI) within 10 min at pH 3, along with excellent cycling stability, outperforming pure ZIS and most previously reported ZIS-based catalysts. The improved photocatalytic activity is attributed to the unique heterostructure and composition of NiCo 2 O 4 @ZIS, where intimate interfacial contact facilitates charge separation and transfer while suppressing charge recombination. Additionally, homogeneous arrangement of ZIS nanosheets over NiCo 2 O 4 raises the quantity of active sites and enhances light harvesting. This study presents a viable strategy for constructing core@shell heterostructured photocatalysts based on ZIS toward highly efficient Cr(VI) reduction.
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高影响因子
Carbohydrate Polymer Technologies and Applications
·
2026
·
IF 7.6
Jiarui Wang,Fan Zhang,Xiaona Huang,Xiaotong Dong,Hang Jiang,Yungang Bai,Kun Xu,Pixin Wang
1 The development of natural polymer-based materials for the efficient and rapid removal of hexavalent chromium (Cr (VI)) from water remains a persistent global challenge. In this study, hyperbranched polyvinylamine (H-PVAm 1 ) was prepared via copolymerization and hydrolysis using N-vinylformamide (NVF) and the branching agent dipentaerythritol hexaallyl ether (DPHAE, 1 wt% relative to NVF) as raw materials. Subsequently, using epichlorohydrin (ECH) as the crosslinking agent, H-PVAm 1 was grafted onto the surface of microcrystalline cellulose (MCC) to obtain the functionalized cellulose adsorbent H-PVAm 1 -MCC. Benefiting from the high primary amine content and three-dimensional branched structure of H-PVAm 1 , H-PVAm 1 -MCC exhibited high primary amine density (19.06 mmol/g), high specific surface area (13.5 m²/g), and good salt resistance. The maximum adsorbed amount of H-PVAm 1 -MCC for Cr (Ⅵ) reached 538 mg/g, which was higher than that of most reported amine-modified cellulose-based adsorbents. Moreover, H-PVAm 1 -MCC exhibited rapid Cr (VI) adsorption kinetics, even at low concentrations (1 ppm). Within 2 min of adsorption, the residual Cr (VI) concentration satisfied the WHO drinking water guideline (≤0.05 ppm). Even in the presence of coexisting ions, H-PVAm 1 -MCC maintained a high Cr (VI) removal rate. Moreover, H-PVAm 1 -MCC exhibited good stability, maintaining 90% adsorbed amount after eight adsorption-desorption cycles. This study provides a strategy for the further development of cellulose-based Cr (VI) adsorbents.
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JOURNAL OF HAZARDOUS MATERIALS
·
2018
·
IF 6.434
Qiang Liu,Qinze Liu,Bingsi Liu,Tao Hu,Weiliang Liu,Jinshui Yao
Newly developed adsorbents, poly(tannin-hexamethylendiamine) (PTHA), were fabricated by varying the mole ratio of tannin (TA) and hexamethylendiamine (HA) under one-pot reaction. The specific forming process of the adsorbent which had undergone the transition from hydrogen bonds to covalent bonds was subsequently explored. Based on the efficiency of Cr(VI) removal from aqueous solution over all prepared adsorbents, the PTHA-4 (mole ratio of TA/HA = 1:12.5) exhibited an excellent adsorption behavior. Adsorption experiments affected by contact time and ionic strength have been conducted successively by PTHA-4, and the equilibrium was reached at 24 h. The kinetic data revealed that the adsorption was good agreement with pseudo-second order model and needed to undergo the rate-controlling step. The maximum adsorption capacity was 283.29 mg/g at 30 °C, relying on the isothermal curve suitably described by Langmuir model. Furthermore, toxic Cr(VI) had been reduced to the low toxic Cr(III) during adsorption process. The structures and adsorption performance of adsorbent were confirmed by means of SEM, FT-IR, XPS etc. Thus, the cheap-sustainable adsorbents have a superior feature for Cr(VI)-wastewater purification in future.
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