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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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.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Haidong Li,Han Song,Yuankun Yang,Haitao Wang,Beibei Fan,Juncheng Zheng,Weiguo Tu,Xuemei Luo,Shu Chen
Efficient and economical reduction and elimination of co-pollution of vanadium (V) and chromium (Cr) from water sources is a major challenge. In this study, sulphate green rust (GR SO4 ) was successfully prepared by co-precipitation method and used for the removal of V(V) and Cr(VI). The findings from batch adsorption experiments indicated that the adsorption capacity of GR SO4 for V(V) and Cr(VI) individually was 30.66 mg⋅g −1 and 39.48 mg⋅g −1 , respectively, with equilibrium reached in 25 min and 10 min. Intriguingly, in a binary system with both V(V) and Cr(VI) present, the time to reach adsorption equilibrium for V(V) removal by GR SO4 was 30 % shorter comparison to the single system under identical conditions. By analyzing the surface characteristics, crystal structure and elemental valence changes of GR SO4 minerals before and after the reaction, it can be obtained that: i) Direct adsorption mainly drives the removal of V(V) by GR SO4 , whereas the removal of Cr(VI) is preceded by reduction and followed by adsorption. ii) In a binary coexistence system, the formation of Fe(III)-Cr(III) oxide (GR-Cr(III)) during the removal of Cr(VI) by GR SO4 formed during the removal of Cr(VI) by GR SO4 creates additional adsorption sites for V(V), which shortens the equilibrium time of the V(V) removal reaction by GR SO4 and reduces the amount of V(V) leached. These findings are of great practical significance for understanding the mechanism and practical application of GR SO4 in the synergistic removal of V(V) and Cr(VI) heavy metals and provide valuable insights into their geophysical-chemical cycling.
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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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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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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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高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Hongbo He,Zhuangzhu Luo,Zhen-Yu Tang,Changlin Yu
Structure controlled ZnWO 4 nanomaterials were fabricated by a facile hydrothermal reaction . The nanorod-like ZnWO 4 with exposed (111) facets exhibits significant promoting effect for Cr 6+ reduction than that of noncrystalline ZnWO 4 nanoparticles . Specifically, the photocatalytic performance of ZnWO 4 -T14 for Cr 6+ reduction is 9.8 times higher than that of ZnWO 4 -T0. The effect of Zn 2+ on the concentration-absorbance (C-A) curve of K 2 Cr 2 O 7 solution was evaluated and investigated systemically, and adding Zn 2+ can improve the UV–vis spectrum detection sensitivity of K 2 Cr 2 O 7 solution. Methylene blue (MB) as a photosensitizer to enhance the photocatalytic activity of ZnWO 4 for Cr 6+ reduction is reported for the first time. In particular, the photocatalytic activity of ZnWO 4 -T14 for Cr 6+ reduction is 96.7% in 10 mg/L MB solution, which is 65.1% higher than that in aqueous solution. Moreover, the ZnWO 4 -T14/MB possesses excellent stability, and the reduction rate of Cr 6+ remains above 90% after four cycles. We believe that the photosensitized strategy is a promising methodology in the treatment of heavy metal ion due to its superior photocatalytic activity and stability.
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高影响因子
WATER ENVIRONMENT RESEARCH
·
2019
·Vol. 91
·期 7
·565-572
·
IF 1.24
Jingge Shang,Jie Gao,Junting Xi,Yingjie Wang,Fangyu Ji,Ruijun Li
A graphene oxide (GO)—nanoscale zerovalent iron (nZVI)—biochar composite (GO-nZVI/BC) was synthesized prior to characterization by X-ray diffraction (XRD), vibrating sample magnetometer (VSM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy analyses. Batch experiments were performed at different initial Cr(VI) concentrations, contact times, and solution pH values. The effects of coexisting anions and chelating agents were also examined. The results indicated that the removal of Cr(VI) was highly pH-dependent and reached a maximum capacity at pH of 2. The equilibrium data were fitted well with the Langmuir isotherm model, and the kinetic data fitted better with the pseudo-second-order kinetic model. The increasing concentrations of EDTA in aqueous solutions were favorable to the removal of Cr(VI), while significantly inhibited adsorption. Furthermore, the GO-nZVI/BC maintained ~84.5% of its original capacity after aging in the air for 25 weeks. Based on the removal efficiency, GO-nZVI/BC can be considered to be an effective material for water treatment applications. Practitioner points Biochar-supported graphene oxide-coated nanoscale zerovalent iron (GO-nZVI/BC) was synthesized and used to treat Cr(VI) from solution. Cr(VI) removal was pH-dependent and obeyed the Langmuir isotherm model and pseudo-second-order model. GO-nZVI/BC maintained ~84.5% of its original capacity after aging for 25 w in the air. Graphical TEM and Magnetic Field of GO-nZVI/BC and its removal capacity of Cr(VI).
研究领域:
环境科学
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材料科学
·
水处理技术
·
污染物修复
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CHEMICAL ENGINEERING & TECHNOLOGY
·
2026
·Vol. 49
·期 6
·e70256
·
IF 2
Yandi Li,Songyi Ji,Rong Zhang,Xiaoling Li,Xiandong Hao,Ning Zhao,Bo Wang,Zhiyong Xu,Wenbo Zhao
Carbon dioxide capture is critical for mitigating climate change. Amine-functionalized MIL-101(Cr) shows great promise due to its high stability and tunable porosity. We optimized its synthesis (160°C, 24 h, 150°C activation) and investigated diethylenetriamine (DETA) loading effects. The 50 wt% DETA composite achieved a CO 2 uptake of 1.25 mmol/g at 30°C and 0.1 bar, nearly six times that of pristine MIL-101(Cr). Kinetic and isotherm data were well described by the pseudo-second-order and Langmuir models. Thermodynamic analysis revealed Δ H = −54.78 kJ/mol and Δ S = −142.13 J/(mol K), confirming an exothermic, chemisorption-dominated process. We further optimized adsorption/desorption conditions, identifying optimal working temperatures of 269.47 K (adsorption) and 388.20 K (desorption). This work provides clear guidance for designing high-performance metal–organic framework (MOF)-based CO 2 capture materials.
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JOURNAL OF POLYMERS AND THE ENVIRONMENT
·
2023
·Vol. 31
·期 7
·2999-3014
·
IF 5.3
Song Jie,Chen Lijun,Niu Yuhua,Wei Zhiqiang,Sun Yonghui
From the perspective of environmental protection, high removal rate, reusable and degradable, amino-functionalized porous hydrogel material P-(EA-β-CD/KHA/AC) was synthesized by introducing ethylamino cyclodextrin, humic acid, and activated carbon, using polyacrylic acid as the carrier. MB and Cr (VI) are common wastewater pollutants, thus, Such contaminants must be removed from the water. The gel materials before and after adsorption were characterized by Fourier transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The removal of MB and Cr(VI) showed high adsorption capacity. At 298 K and pH 8, the adsorption capacities of P-(EA-β-CD/KHA/AC) hydrogel for MB and Cr(VI) were as high as 262.31 and 170.12 mg/g, respectively, and the removal rates were 98.96% and 70.27%, respectively. The adsorption behavior follows the pseudo-second-order kinetic equation, conforming to the Langmuir model; and through intermolecular forces, π–π conjugation, chelation, and other interactions, entropy-increasing, endothermic, and spontaneous process is formed. The regeneration and degradability experiments of P-(EA-β-CD/KHA/AC) hydrogel were conducted and its recycling performance was verified.
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