CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Peng Hu,Xiaopeng Liang,Muhammad Yaseen,Xiaodan Sun,Zhangfa Tong,Zhongxing Zhao,Zhenxia Zhao
A novel mechano-chemical strategy using dopamine to modify UiO-66(Zr) by N-coordination was proposed to enhance its competitive adsorption for acetaldehyde, chlorobenzene/H 2 O, both thermodynamically and kinetically. The newly synthesized material was characterized by SEM, EDX, XPS, PXRD, FT-IR, TGA/DTG and BET techniques. Results showed that N was successfully grafted into UiO-66(Zr) frameworks through coordination interaction with Zr-O clusters resulting in M-UiO-66(Zr-N 3.0 ). The obtained M-UiO-66(Zr-N 3.0 ) exhibited a significant increase in adsorption of chlorobenzene (4.94 mmol/g) and acetaldehyde (9.42 mmol/g) compared to parent UiO-66(Zr) and UiO-66(Zr)-NH 2 . The H 2 O adsorption uptake of M-UiO-66(Zr-N 3.0 ) decreased by 20% that of UiO-66(Zr) and 47% of UiO-66(Zr)-NH 2 indicating higher hydrophobicity of the modified material. Kinetic performance indicated that diffusivity of chlorobenzene on M-UiO-66(Zr-N 3.0 ) was about 7.8 and 40 times higher than that of the parent UiO-66(Zr) and UiO-66(Zr)-NH 2 respectively and 15.4 times higher than that of H 2 O on itself. Based on the results, the current N-modification strategy can be deemed as an efficient way to improve MOFs competitive adsorption towards VOCs under humid conditions and it might play active role in industries involving adsorbent applications.
研究领域:
材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2025
·
IF 4.7
Jianglu Teng,Xibin Shen,Guohua Hang,Yuan Gao,Jiawei Hu,Sixun Zheng
The reaction of 4-(hydroxymethyl)phenylboronic acid with triethanolamine was carried out to synthesize a boronic ester diol featuring boron–nitrogen (B–N) coordination. This diol served as a chain extender, allowing B–N-coordinated boronic ester bonds to be introduced into polyurethane (PU) networks. Toward this end, we first synthesized a series of α,ω-dihydroxyl polyurethane telechelics with α,ω-dihydroxypropyl poly(dimethylsiloxane) as the polymeric diol. By varying the molar ratio of the boronic ester diol to 1,4-butane diol, the α,ω-dihydroxyl polyurethane telechelics were synthesized with variable contents of the dynamic covalent bonds. Thereafter, the reaction of α,ω-dihydroxyl PU telechelics with 3-isocyanatopropyl triethoxysilane was carried out to gain α,ω-ditriethoxysiloxane PU telechelics. The latter were readily cross-linked via the sol–gel process to afford the mechanically robust PU networks, with Young’s modulus and tensile strength as high as 302.7 and 35.4 MPa, respectively. More importantly, the reprocessing properties were imparted to the PU networks. Compared to the control PU network, the reprocessing temperature was depressed to 120 °C. In the meantime, the shape memory properties of PU networks were significantly improved through the introduction of dynamic covalent bonds. Furthermore, the shape memory networks featured reconfigurability with the introduction of B–N-coordinated boronic ester bonds.
研究领域:
材料科学
·
高分子化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2022
·
IF 4.331
Tongtong Pan,Gan Li,Rujie Li,Xiangmei Cui,Weidong Zhang
The remediation of environmental boron contamination has received extensive research attention. The adsorbent ECH@NGM aerogel with high hydrophilic and mechanical properties was synthesized to remove boron. The ECH@NGM aerogel had a high adsorption capacity of 81.11 mg/g, which was 14.50% higher than that of commercial boron-selective resin Amberlite IRA743. The Freundlich model and pseudo-second-order model described the adsorption behavior well. In addition, the response surface methodology (RSM) could predict the experimental outcomes and optimize the reaction conditions, and X-ray photoelectron spectroscopy (XPS) and control tests were utilized to investigate probable adsorption mechanisms. These data showed that the B ← N coordination bond was the primary adsorption force. The adsorbent had good resistance to interference from coexisting salts, high reusability, good adsorption performance even after five reuse cycles, and a high desorption rate in a relatively short time. The adsorption performance in real brines could be maintained at 80%. Therefore, this work not only provided ECH@NGM aerogels for the removal of boron from brine but also elucidated the main adsorption processes between N-containing adsorbents and boron, facilitating the design of future adsorbents for boron removal.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Hongchao Li,Jieshu Qian,Bingcai Pan
Co-based carbonaceous materials are among the most effective heterogeneous catalysts to activate peroxymonosulfate (PMS) for the degradation of organic pollutants in water. However, present examples normally suffer the aggregation of catalyst and/or the leakage of active Co species especially when the Co content is high, resulting in a loss of reactivity and potential environmental risk. In this study, we report the use of a mixture of Co phthalocyanine and melamine as precursor for the preparation of a carbonaceous catalyst with N-coordinated Co (Co-NG) for PMS activation . The presence of Co phthalocyanine in the precursor facilitates the uniform distribution of Co species in carbonaceous substrate with high Co content of 8.0 wt%, thus exhibiting remarkable catalytic reactivity for the degradation of a variety of organic pollutants. More importantly, the strong coordination by N atoms significantly enhances the Co stability and reduces the Co leaching during cyclic use. Experiment results demonstrate that both sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO • ) contribute to the pollutant degradation with SO 4 •− as the main reactive species. Other reaction parameters including solution pH, the presence of inorganic anions, and natural organic matters were also investigated and evaluated. We reckon this study provides new insights for the design of efficient Co-based carbonaceous catalysts with high Co stability for water treatment application.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Jingjing He,Yu Wan,Wenjun Zhou
Developing high-efficient hybrids carbon catalysts for PMS-based advanced oxidation process (AOPs) are crucial in the field of environmental remediation. In this work, novel carbon nanocubes (xFe‒N‒C) with three-dimensional porous structure and abundant well-dispersed FeN x sites were obtained via a skillful cage-encapsulated-precursor pyrolysis strategy. The as-synthesized xFe‒N‒C exhibited superb activity for phenol degradation by activating peroxymonosulfate (PMS). Besides, the catalytic system not only possessed good recycling performance, wide pH adaptation and relatively low activation energy, but also had high resistance to environmental interference. Singlet oxygen ( 1 O 2 ) dominated non-radical process was responsible for phenol degradation rather than traditional radical pathways. Impressively, the doping level of Fe could regulate FeN x contents in catalysts, and the catalytic activity of xFe‒N‒C was greatly enhanced with increasing FeN x contents. Based on density functional theory calculations (DFT), the introduction of FeN x sites regulated the electronic structure of catalysts. Such electron-deficient Fe center acted as electron acceptor to receive electrons transmitted by the adsorbed PMS , thus generating highly reactive 1 O 2 for rapid phenol oxidation. This work provides a new insight into the innovation in transition metal-nitrogen hybrid carbon catalysts and highlights the pivotal roles of FeN x sites in 1 O 2 generation during PMS activation process.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF SEPARATION SCIENCE
·
2018
·Vol. 42
·期 4
·878-887
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IF 2.415
Jiangyi Wu,Meng Mei,Xiaojia Huang
To enrich carbamate pesticides from complex matrices, an adsorbent based on poly (vinylboronic anhydride pyridine complex- co -ethylenedimethacrylate) monolith was fabricated and utilized as the extraction phase of multiple monolithic fiber solid-phase microextraction. Due to the abundant boron atoms in the monolith, the B–N coordination interaction between adsorbent and analytes play a key role in the efficient extraction of analytes. Under the optimized conditions, the monolithic fibers were combined with high-performance liquid chromatography for the quantify trace levels of carbamate pesticides in environmental water and orange juice samples. For water sample, the limit of detection and limit of quantification were in the range of 0.017–0.29 and 0.057–0.96 μg/L, respectively. The related values in orange juice samples were 0.038–0.39 and 0.12–1.36 μg/kg, respectively. Besides, the proposed method also exhibits wide linearity, satisfactory coefficients of determination, and good precision. The introduced approach was successfully applied to determine trace target analytes in real-life samples. The spiked recoveries with different fortified concentrations were in the range of 80.4–117% for water samples and 83.7–119% for fruit juice samples. The relative standard deviations were below 10%. The results evidence that the suggested method was convenient, reliable, and eco-friendly for the monitoring of trace levels of carbamate pesticides in complex samples such as waters and juices.
研究领域:
分析化学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2020
·Vol. 7
·期 5
·1298-1306
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IF 5.958
Xiugang Li,Chunling Zhang,Minghong Luo,Qilu Yao,Zhang-Hui Lu
Nitrogen-rich covalent organic frameworks (COFs) with a high content of nitrogen and an inherent porous skeleton are considered as a remarkable support for encapsulating active metal nanoparticles (MNPs). Herein, a cost-effective and nitrogen-rich COF (PC-COF) synthesized from piperazine and cyanuric chloride was used as a carrier for encapsulating Rh NPs via a metal–nitrogen (M–N) coordination reduction strategy. Numerous precisely tailored N atoms within the PC-COF facilitate the construction of Rh–N complexes between Rh ions and N atoms, which can be in situ reduced to produce ultrafine Rh NPs confined in the pores of the PC-COF. The optimized Rh/PC-COF catalyst shows uniform dispersibility and a fairly narrow distribution (1.4–2.6 nm) of Rh NPs, giving an ultrahigh catalytic activity for the methanolysis of ammonia borane (AB) with a total turnover frequency (TOF) of 505 min−1 at 298 K. The excellent catalytic performances can be ascribed to the ultrafine particle size, electronic-rich Rh NPs, and the synergistic effect of the Rh NPs and PC-COF. The M–N coordination reduction strategy for encapsulating ultrafine MNPs into the pores of COFs opens a valuable pathway for developing metal nanocatalysts with high catalytic performance and excellent stability.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
ADVANCED MATERIALS
·
2025
·
IF 26.8
Boyu Wang,Yani Huo,Cheng Chen,Xiao-Ye Wang,Chuancheng Jia,Jinying Wang,Xuefeng Guo
Achieving dynamic control over stereostructures and electronic properties of rigid molecules remains a significant challenge due to the delicate balance between stability and flexibility. Here, the construction of butterfly-shaped molecular junctions stabilized by moderate-strength boron-nitrogen (B←N) coordination between boraacenes and pyridines is reported. By leveraging the pivot-like flexibility of B←N bonds, molecular conductance switching with on/off ratios exceeding 100 is achieved through force-driven dynamic transitions between distinct stacking conformations. Single-molecule electrical measurements combined with first-principle calculations identify distinct charge transport mechanisms—through-space and through-bond—associated with the butterfly-wing open and closed configurations. Furthermore, external factors like electric fields and substituent effects modulate π – π interactions and charge transport properties. The introduction of destructive quantum interference effects can be achieved by replacing molecular units. The findings demonstrate that B←N coordination serves as a dynamically tunable linkage, offering a pathway to design molecular platforms with multifunctional units, customized stereo-conformations, and quantum effects.
研究领域:
物理化学
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分子电子学
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超分子化学
·
纳米科技
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材料科学
·
理论计算化学
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有机功能材料
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化学生物学
✓ 已验证
DOI
PubMed
高影响因子
POLYMER DEGRADATION AND STABILITY
·
2025
·
IF 7.4
Xuebin Lian,Yuanjian Li,Minghui Li,Yongxin Bai,Xinyu Zhao,Jiangwen Li,Shujun Zhao
Achieving simultaneous exceptional adhesion and recyclability remains a formidable challenge due to the inherent strength-toughness trade-off and stability-switchability conflict in adhesive systems. Inspired by the hierarchical architecture of cartilage, we report a bioinspired cross-linked network integrating B-N coordination bonds and dynamic boronic ester linkages for high-performance recyclable adhesives. The biomimetic design replicates the structural organization of cartilage's collagen-proteoglycan matrix, where dynamic B-N coordination bonds between network junctions facilitate energy dissipation through bond dissociation-induced network elongation. The network is constructed via 3-amino-1,2-propanediol-mediated epoxy ring-opening and subsequent cross-linking with 1,4-phenylenediboronic acid, forming a dynamic covalent polymer network, denoted as BEAD (boronic ester adhesive), with high cross-linking density. BEAD exhibits exceptional mechanical properties (46.42 ± 5.32 MPa tensile strength, 2.60 ± 0.31 MJ/m³ toughness) and robust adhesion (26.69 ± 0.74 MPa lap shear strength on steel). The synergy of B-N coordination (enhancing cohesion) and boronic ester exchange (enabling reprocessability) yields an optimal balance of strength and recyclability, retaining 80.7% adhesion performance after five reprocessing cycles. The study presents a biomimetic dynamic bonding strategy to overcome the strength-recyclability trade-off in adhesives, establishing a sustainable paradigm for structural materials.
研究领域:
高分子材料科学
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生物仿生工程
·
粘附力学
·
可持续材料
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功能高分子
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界面化学
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结构胶黏剂
✓ 已验证
产品关联
DOI
高影响因子
Energy & Environmental Science
·
2024
·Vol. 17
·期 14
·5227-5240
·
IF 32.4
Changle Yue,Chao Feng,Guangxun Sun,Na Liu,Haoyuan Hao,Wenjing Bao,Xiaowei Zhang,Fengyue Sun,Cong Zhang,Jiahui Bi,Yan Zhou,Hsiao-Chien Chen,Yuan Pan,Daofeng Sun,Yukun Lu
Tuning and stabilizing the chemical microenvironment of Pt-based single-atom catalysts is a major challenge in promoting an electrocatalytic hydrogen evolution reaction (HER). Herein, we constructed a hierarchical stabilization system of Pt single-atoms via defect substitution using the polyoxometalate (POM) (NH4)4[ZnMo6O24H6] (ZnMo6) as a template. The well-defined structure of ZnMo6 led to precise local Zn sublimation during the formation of Mo2C, which was converted from the Mo6 ring in situ. The localized defect provides a well-defined Mo(C)–Pt–N coordination environment to trap Pt single-atoms. The obtained single-atom catalyst (PtSA@Mo2C@NC) exhibited a superior and stable electrochemical HER performance with an unprecedented mass activity of 75.21 A mgPt−1 in 0.5 M H2SO4. In-depth theoretical calculation analysis revealed that Mo(C)–Pt–N coordination provides a moderated charge state and low d-band center of the Pt site, thus significantly promoting proton adsorption and H2 desorption. This work demonstrates a promising single-atom stabilization strategy for constructing high-performance HER electrocatalysts through the precise modulation of a three-dimensional chemical environment.
研究领域:
材料科学
·
电化学
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 9
·1416
·
IF 5.719
Yining Jia,Rong Huang,Ruijuan Qi
Numerous efforts have been devoted to realizing the high loading and full utilization of single-atom catalysts (SACs). As one of the representative methods, atom migration-trapping (AMT) is a top-down strategy that converts a certain volume of metal nanoparticles (NPs) or metal-based precursors into mobile metal species at high temperature, which can then be trapped by suitable supports. In this study, high-loading iron single atoms anchored onto carbon matrix/g-C3N4hybrid supports were obtained through a single-atom migration-trapping method based on metal–organic framework (MOF) pyrolysis. It is confirmed, by high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM), X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS), that the Fe(acac)3precursor is reduced to Fe single atoms (SAs), which are not only anchored onto the original N-doped carbon (NC), but also onto g-C3N4, with an Fe-N coordination bond. Further electrochemical results reveal that Fe-C3N4-0.075 possesses a better half-wave potential of 0.846 V and onset potential of 0.96 V compared to Fe-N-C, the product obtained after pyrolysis of Fe(acac)3@ZIF-8. As opposed to SAs prepared by the pyrolysis process only, SAs prepared by AMT are commonly anchored onto the surface of the supports, which is a simple and effective way to make full use of the source metal and prepare SACs with higher exposing active sites.Keywords:atom migration-trapping;single-atom catalysts;metal–organic frameworks
研究领域:
催化
·
材料科学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Ling Hu,Zhiwen Wang,Yingzhang Shi,Cheng Liu,Yidong Hou,Jinhong Bi,Ling Wu
The defect-rich ultrathin WO 3 nanosheets are successfully prepared as photocatalysts via heating treatment for the pristine WO 3 nanosheets (NS) in vacuum (NSV) and N 2 atmosphere (NSN). The increment of degradation efficiencies of levofloxacin (LVX) over NS (49.9 %)
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）