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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Facile fabrication of phenylenediamine residue derived N, O co-doped hierarchical hyperporous carbon for high-efficient chloroxylenol removal

Wen-Long Yu,Shi-Lei Zhao,Guang-Wen Xu,Xin Li,Xiao-Lei Zhang,Yu-Ling Shan,Jun-Wei Ding,Guo-Hui Qin,Jun-Mei Zhang,Xiang Feng,De Chen

The chloroxylenol (PCMX) has shown well virucidal efficacy against COVID-19, but the large-scale utilization of which will undoubtedly pose extra environmental threaten. In the present study, the recycled industrial phenylenediamine residue was used and an integrated strategy of “carbonization-casting-activation” using super low-dose of activator and templates was established to achieve in-situ N/O co-doping and facile synthesis of a kind of hierarchical hyperporous carbons (HHPC). The sample of HHPC-1.25–0.5 obtained with activator and template to residue of 1.25 and 0.5 respectively shows super-high specific surface area of 3602 m 2 /g and volume of 2.81 cm 3 /g and demonstrates remarkable adsorption capacity of 1475 mg/g for PCMX in batch and of 1148 mg/g in dynamic column adsorption test. In addition, the HHPC-1.25–0.5 exhibits excellent reusability and tolerance for PCMX adsorption under various ionic backgrounds and real water matrix conditions. The combined physio-chemistry characterization, kinetic study and DFT calculation reveal that the enhanced high performances originate from the hierarchical pore structure and strong electrostatic interaction between PCMX and surface rich pyridinic-N and carbonyl groups.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI 高影响因子
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ACS Applied Nano Materials · 2024 · IF 5.3

Ni2P Nanoparticles Supported on N, P Co-Doped Carbon as Catalyst for α-Alkylation of Arylacetonitriles with Alcohols

Tianyue Su,Junsheng Wang,Chun Cai

The nickel phosphides have garnered increasing attention as an excellent catalytic site in the fields of electrocatalysis and hydrotreating, but their application in organic synthesis remains infrequent. In this study, ammonium phosphate and nickel chloride were employed as the doping sources for the first time to synthesize the Ni-based ZIF-8 precursor via the host–guest method. Subsequently, the precursor was pyrolyzed to obtain Ni2P nanoparticles (NPs) supported on N, P co-doped carbon. The composite materials exhibit elevated metal loading and effective dispersion due to the synergistic combination of phosphorus and nickel. Specifically, compared with Ni-NC, the optimal Ni2P-NCP-1 exhibits enhanced catalytic activity in the α-alkylation of arylacetonitriles with alcohols using KOH as the base. It shows a wide broad substrate scope at 140 °C for 12 h in n-octane using a hydrogen borrowing strategy. Through characterizations and mechanistic studies, it has been discovered that the introduction of P source not only provides more basic sites on carbon matrix but also leads to the formation of Ni2P NPs, which facilitates the catalytic efficiency by modifying the electronic structure of Ni. Compared with the metallic Ni species, the synergistic effect between Ni2P and acid-basic sites significantly influences the dehydrogenation of alcohols to generate Ni–H species. This study successfully achieves simultaneous phosphating of both the metal and support, and it also demonstrates that the N2P-NCP-1 catalyst has significant potential in the heterogeneous organic transformation field.

研究领域: 有机化学 · 材料科学 · 催化反应
✓ 已验证 DOI 高影响因子
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CHINESE JOURNAL OF CATALYSIS · 2021 · IF 8.271

N-doped carbon-coated Fe3N composite as heterogeneous electro-Fenton catalyst for efficient degradation of organics

Juan Xiao,Junwei Chen,Zuqiao Ou,Junhang Lai,Tongwen Yu,Yi Wang

Herein, the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework (Fe 3 N@NG/NC) is investigated as a heterogeneous electro-Fenton (HE-EF) catalyst for the efficient removal of organics. The simultaneous carbonization and ammonia etching of iron-based metal organic framework (Fe-MOF) materials yielded well-dispersed N-doped carbon-coated Fe 3 N nanoparticles with a diameter of ~70 nm. The Fe 3 N and pyridinic N endowed the composite with high HE-EF activity for decomposing the electrogenerated H 2 O 2 to • OH. The Fe 3 N@NG/NC exhibited outstanding HE-EF performance in removing various organic pollutants with low iron leaching. A removal rate of 97–100% could be obtained for rhodamine B (RhB), dimethyl phthalate , methylene blue , and orange II in 120 min at a pH of 5.0. When the solution pH was set to 3.0, 5.0, 7.0, and 9.0, the removal rate of RhB reached 100%, 96%, 92%, and 81%, respectively, in 60 min at an optimum voltage of 0.0 V ( vs. reversible hydrogen electrode (RHE)). Moreover, the concentration of leached iron was expected to be below 0.03 mg/L in a wide pH range of 3.0–9.0. In addition, the RhB removal efficiency remained as high as 90% after six cycles in the reusability experiments. This work highlights the MOF-derived Fe 3 N composite as an efficient HE-EF catalyst and the corresponding catalytic mechanism, which facilitates its application in wastewater treatment .

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI 高影响因子
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Applied Catalysis O: Open · 2024 · IF 0

P-N bonds in P-modified biochar/g-C3N4 composite constructed via mechanochemical method to enhance photodegradation of indigo carmine

Yongsi Jiao,Cunjun Li,Yanqi Xu,Limei He,Linjiang Wang

Photodegradation of indigo carmine (IC) in wastewater has received much attention in recent decades. However, the current photocatalysts used for IC photodegradation suffer from an unsatisfactory efficiency due to low yield of reactive species. Herein, a P-modified biochar/g-C 3 N 4 (P-BC/CN) photocatalyst was fabricated by mechanochemical method using P-modified biochar and g-C 3 N 4 as precursors. It is discovered that P N bonds were constructed between P-modified biochar and g-C 3 N 4 , and these bonds served as the active sites to promote the generation of •O 2 − during the photodegradation process. The biochar component in P-BC/CN composite is conducive to transfer the photogenerated carriers, thereby avoiding their recombination. The photodegradation experiment showed that the P-BC/CN composite exhibits an impressive photodegradation performance towards IC ( C 0  = 50 mg/L) with a photodegradation rate of 95.3% in 120 min. This work provides a green and efficient method to design biochar-based photocatalyst with P N active sites for advanced wastewater purification.

研究领域: 环境科学 · 材料科学 · 化学工程
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY · 2015 ·Vol. 15 ·期 6 ·4608-4618 · IF 1.556

Superparamagnetic Fe3O4/Poly(N-isopropyl acrylamide) Nanocomposites Synthesized in Inverse Miniemulsions: Magnetic and Particle Properties

Cui Qinmin,Zhu Shudi,Yan Yingjie,Ye Quanlin,Ziener Ulrich,Cao Zhihai

In the present study, superparamagnetic Fe3O4/poly(N-isopropyl acrylamide) nanocomposites were synthesized by one-step inverse miniemulsion copolymerization of N-isopropyl acrylamide and N,N'-methylene diacrylamide. The loading of Fe3O4 nanoparticles in the nanocomposites was 27 wt%, and the saturation moment of the nanocomposites was 12.4 emu · g−1. Fe3O4 nanoparticles were prepared through a coprecipitation method. The amount of stabilizer (poly(acrylic acid)) significantly influenced the size and size distribution of the Fe3O4 nanoparticles, and, therefore, their magnetic properties. Superparamagnetism of the Fe3O4 nanoparticles was preserved in the nanocomposites. The effects of synthetic parameters on the particle properties, namely surfactant loading, concentration of ferrofluid, type of lipophobe and initiator, and amount of cross-linker were investigated. Nanocomposites of Fe3O4/poly(N-isopropyl acrylamide) displayed a guava-like morphology, which they could retain after being redispersed in polar solvents.

研究领域: 材料科学 · 纳米技术 · 化学工程
✓ 已验证 DOI 高影响因子
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ChemSusChem · 2020 ·Vol. 13 ·期 16 ·4151-4158 · IF 7.962

Oxidative Esterification of 5-Hydroxymethylfurfural with an N-doped Carbon-supported CoCu Bimetallic Catalyst

Huai Liu,Ning Ding,Junnan Wei,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Huayu Fang,Tianyuan Li,Lu Lin

Graphical No base needed : N-doped carbon-supported CoCu bimetallic catalyst with enhanced O 2 activation ability and basicity is demonstrated as an effective catalyst for the oxidative esterification of 5-hydroxymethylfurfural. The introduction of Cu significantly enhances the catalytic activity, resulting in a high furan-2,5-dimethylcarboxylate yield and an impressive formation rate, paving the way for the efficient and green synthesis of sustainable bio-based polymer monomers. The direct fabrication of furan-2,5-dimethylcarboxylate (FDMC), a promising renewable monomer, from biomass-derived 5-hydroxymethylfurfural (HMF) is a cutting-edge process. In this contribution, an elaborately designed N-doped carbon-supported CoCu bimetallic catalyst (Co x Cu y -NC; x / y= 9:1, 7:3, 4:6, which represents the designed molar ratio of Co and Cu in the catalyst), which could offer a desirable FDMC yield of 95 % under mild and base-free conditions (Co 7 Cu 3 -NC, 2 bar O 2 , 80 °C, 4 h) is described for the oxidative esterification of HMF. Notably, an FDMC formation rate of 6.1 mol FDMC mol Co −1 h −1 was achieved over Co 7 Cu 3 -NC, which represents the highest catalytic efficiency so far among Co-based catalytic systems. It has been demonstrated that Cu-doping in Co 7 Cu 3 -NC catalyst brings about more active sites (Co-N x species) with stronger molecular oxygen activation ability. The increase of surface N content of Co 7 Cu 3 -NC also improves basicity of the catalyst, which favors the hydrogen abstraction process during the HMF oxidative esterification reaction. These findings may pave an efficient and green way for the synthesis of sustainable bio-based polymer monomers.

研究领域: 催化化学 · 生物质转化 · 绿色化学
✓ 已验证 DOI 高影响因子
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Template-Oriented Synthesis of Fe–N-Codoped Graphene Nanoshells Derived from Petroleum Pitch for Efficient Nitroaromatics Reduction

Tianwen Ma,Xiaojie Tan,Qingshan Zhao,Zhuangzhuang Wu,Fengliang Cao,Jingyan Liu,Xiaocui Wu,Hui Liu,Xiaobo Wang,Hui Ning,Mingbo Wu

In this study, we demonstrate noble metal-free Fe–N-codoped graphene nanoshells (Fe–N/GNS) derived from petroleum pitch as highly efficient and cost-effective catalysts for nitroaromatics reduction. By employing α-Fe2O3 nanoparticles simultaneously as both the hard template and the metal source, Fe–N/GNS can be facilely synthesized through the template-oriented method, followed by thermal annealing with urea for nitrogen doping. Owing to the high-dispersed synergetic Fe–N active sites as well as the hierarchical porous nanoshell structure, the Fe–N/GNS catalysts show remarkable catalytic performance and good tolerance for the reduction of nitroaromatics with NaBH4 aqueous solution. The optimized Fe–N/GNS-800 corresponds to pseudo-first-order kinetics for p-nitrophenol reduction at room temperature, with the rate constant (k) reaching 1.23 min–1. The reinforced structure also allows the catalyst to be readily recycled a dozen times without activity deterioration. This work may provide a new avenue to facilely fabricate cost-effective but powerful catalysts for nitroaromatics reduction and beyond.

研究领域: 材料科学 · 催化化学 · 环境化学
✓ 已验证 DOI 高影响因子
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Cascading Detection of Hydrogen Sulfide and N-Acetyltransferase 2 in Hepatocellular Carcinoma Cells Using a Two-Photon Fluorescent Probe

Yani Liu,Xueao Wang,Zheng Li,Liping Chen,Xinyi Cai,Zhigang Sun,Wei Cheng,Xiangjie Luo,Hai-Liang Zhu,Yong Qian

Hydrogen sulfide (H2S), a critical gas signaling molecule, and N-acetyltransferase 2 (NAT2), a key enzyme in drug metabolism, are both known active biomarkers for liver function. However, the interactions and effects of H2S and NAT2 in living cells or lesion sites remain unknown due to the lack of imaging tools to achieve simultaneous detection of these two substances, making it challenging to implement real-time imaging and precise tracking. Herein, we report an activity-based two-photon fluorescent probe, TPSP-1, for the cascade detection of H2S and NAT2 in living liver cells. Continuous conversion from TPSP-1 to TPSP-3 was achieved in liver cells and tissues. Significantly, leveraging the outstanding optical properties of this two-photon fluorescent probe, TPSP-1, has been effectively used to identify pathological tissue samples directly from clinical liver cancer patients. This work provides us with this novel sensing and two-photon imaging probe, which can be used as a powerful tool to study the physiological functions of H2S and NAT2 and will help facilitate rapid and accurate diagnosis and therapeutic evaluation of hepatocellular carcinoma.

研究领域: 生物化学 · 医学影像学 · 肿瘤学
✓ 已验证 DOI PubMed 高影响因子
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ChemPlusChem · 2024 · IF 3

Metal-free Regioselective Direct C(4)–H Amination of Quinazoline with N-fluorobenzenesulfonimide

Yong Wang,Xueying Lin,Xianyu Ying,Shan Hu,Hongjun Zhu

A facile C–H amination of quinazoline employing N-fluorobenzenesulfonimide (NFSI) as the amination source has been disclosed in the absence of any metal, oxidant or additive. The methodology shows a board range of quinazolines with different functional groups in moderate to good yields up to 87%. Furthermore, gram-scale reaction, desulfonylation to amine and synthesis of pharmaceutical intermediate were also investigated, which demonstrates potential applications in medicinal chemistry. A plausible amination mechanism is proposed via F+ transfer accompanied by the removal of one molecule of PhSO2F. DFT studies with experimental work suggest that the mechanism via F+ transfer is more favorable than the free radical one.

研究领域: 有机化学 · 药物化学 · 合成化学
✓ 已验证 DOI PubMed 高影响因子
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TALANTA · 2015 · IF 3.545

Development of N-ferrocenyl(benzoyl)amino-acid esters stationary phase for high performance liquid chromatography

Xiaohua Zhou,Xiaole Li,Aijuan Cao,Qiao Lijun,Ajuan Yu,Shusheng Zhang,Yangjie Wu

A new stationary phase for high-performance liquid chromatography was prepared by covalently bonding N-ferrocenyl(benzoyl)amino-acid esters (L 1 ) onto silica gel using 3-aminopropyltriethoxysilane as coupling reagent. The structure of new material was characterized by infrared spectroscopy , elemental analysis and thermogravimetric analysis . The chromatographic behavior of the phase was illustrated in reversed-phase (RP) and normal-phase (NP) modes using polycyclic aromatic hydrocarbons (PAHs), aromatics positional isomers, amines, 5-nitroimidazoles, organophosphorus pesticides and phenols as probes. Multiple mechanisms including hydrophobic, hydrogen bonding , π–π, dipole–dipole, charge-transfer and acid–base equilibrium interactions are involved. Thus, multi-interaction mechanisms and mixed-mode separation of the new phase can very likely guarantee its excellent chromatographic performance for the analysis of complex samples. The L 1 AminoSil column was successfully employed for the analysis of organophosphorus pesticides in vegetable.

研究领域: 分析化学 · 色谱技术
✓ 已验证 DOI 高影响因子
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Small · 2024 ·Vol. 20 ·期 45 ·2403852 · IF 13

Enhanced Thermoelectric Performance of N-Type PbSe Through Semi-Coherent Nanostructure by AgCuTe Alloying

Xinxin Wang,Chao Wang,Yajing Wang,Min Hao,Shengqiang Cui,Xudong Huang,Chunhui Wang,Jing Chen,Zhenxiang Cheng,Jianli Wang

N-type PbSe thermoelectric materials encounter challenges in improving the power factor due to the single-band structure near the Fermi level, which obstructs typical band convergence. The primary strategy for enhancing the thermoelectric figure of merit (ZT) for n-type PbSe involves reducing lattice thermal conductivity (κ lat ) by introducing various defect structures. However, lattice mismatches resulting from internal defects within the matrix can diminish carrier mobility, thereby affecting electrical transport properties. In this study, n-type AgCuTe-alloyed PbSe systems achieve a peak ZT value of ≈1.5 at 773 K. Transmission electron microscopy reveals nanoprecipitates of Ag 2 Te, the room temperature second phase of AgCuTe, within the PbSe matrix. Meanwhile, a unique semi-coherent phase boundary is observed between the PbSe matrix and the Ag 2 Te nanoprecipitates. This semi-coherent phase interface effectively scatters low-frequency phonons while minimizing damage to carrier mobility. Additionally, the dynamic doping effect of Cu atoms from the decomposition of AgCuTe within the matrix further optimize the high-temperature thermoelectric performance. Overall, these factors significantly enhance the ZT across the whole temperature range. The ZT value of ≈1.5 indicates high competitiveness compared to the latest reported n-type PbSe materials, suggesting that these findings hold promise for advancing the development of efficient thermoelectric systems.

研究领域: 材料科学 · 凝聚态物理 · 能源材料 · 纳米结构工程 · 热电转换
✓ 已验证 DOI 高影响因子
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JOURNAL OF CHEMICAL THERMODYNAMICS · 2022 · IF 3.269

Measurement of the speed of sound in near-critical n-dodecane at temperatures from (433 to 679) K and pressures up to 10.0 MPa

Xin Li,Taotao Zhan,Yongbo Zhang,Yuqi Su,Maogang He,Ying Zhang

As one of higher n -alkanes, n -dodecane is an important component of surrogate fuels for aviation kerosene, of which the accurate knowledge of its thermophysical properties is necessary for industrial application. The speed of sound in n -dodecane was measured by the Brillouin light scattering (BLS) in the vicinity of the critical point, of which the examined regions are T = (433.49 to 678.84) K along seven isobaric lines at p = (1.85, 2.0, 2.2, 4.0, 6.0, 8.0, and 10.0) MPa. The relative expanded uncertainty of BLS experimental system is estimated to be less than 1.2% with the confidence level of 95% (coverage factor, k  = 2). Polynomial representations for the speed of sound in liquid n -dodecane was fitted by the experimental results, and the average absolute deviation and maximum absolute deviation are 0.70% and 1.96%, respectively. Moreover, the accuracy of the multiparameter equation of state proposed by Lemmon were assessed by the experimental speeds of sound in the whole investigated p - T region.

研究领域: 化学工程 · 物理化学
✓ 已验证 DOI 高影响因子
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