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CATALYSIS TODAY · 2024 · IF 5.2

Cobalt and nitrogen co-modified graphitic carbon: A bifunctional catalyst for thermocatalytic and electrocatalytic oxidation of HMF to FDCA

Yang Gao,Shilin Fan,Bin Zhu,Soliman I. El-Hout,Jinghui Lyu,Jian Zhang,Chunlin Chen

Biomass energy has gained significant attention due to its renewability and clean, low-carbon characteristics. We prepared a Co@NC-a catalyst using the complexation-carbonation-acid etching method, which can catalyze both thermochemical and electrochemical HMF selective oxidation reactions. In thermocatalysis, it can achieve 100 % HMF conversion and 94.4 % FDCA yield at 65 °C and 0.2 MPa O 2 . In electrocatalysis , 100 % HMF conversion and 73 % FDCA yield were also realized. Significantly, graphitized carbon contributes to the aerobic oxidation of HMF due to its excellent electrical conductivity , which promotes electron transfer during the reaction. Additionally, a comparative study of the activation energy of this catalytic system in electrocatalysis and thermocatalysis showed that electrocatalysis is kinetically more favorable. The energy efficiency calculation also indicates electrocatalysis is more energy efficient than thermocatalysis.

研究领域: 生物质能 · 催化化学 · 材料科学
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ACS Applied Polymer Materials · 2022 · IF 4.855

Detection and Removal of Mercury Ions in Water by a Covalent Organic Framework Rich in Sulfur and Nitrogen

Chunming Tang,Yuancheng Qin,Cailing Ni,Jianping Zou

Hg/Hg(II) is deemed to be the most toxic heavy metal to humans. Therefore, designing suitable adsorbents to simultaneously achieve high capacity, rapid mercury adsorption, and fluorescence detection is still an important challenge in overcoming Hg2+ pollution. Here, we report a flexible alkylamine covalent organic framework (TpTSC), which has been used as an efficient adsorbent and achieves the dual-functional application of TpTSC for Hg2+, with a fluorescence detection limit of 2 ppm and simultaneously a removal capacity of 1035 mg g–1. It can remove 10 ppm mercury solution to below 2 ppb (drinking water standard) within 10 min, and the removal rate is as high as 99.98%. To a certain extent, it exceeds the recently reported thioether or thiol functionalized adsorbents. The kinetic study shows that TpTSC displays a very high Kd value, with Kd = 1.2 × 109 mL g–1, which has a strong affinity for mercury. In addition, TpTSC displays a good recycling capacity, with a removal rate of over 90% after five cycles. In conclusion, sulfur modification is a useful strategy for developing dual-functional COFs to simultaneously remove and detect toxic heavy metal ions.

研究领域: 环境科学 · 材料科学 · 化学工程
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Journal of Materials Chemistry A · 2021 ·Vol. 9 ·期 39 ·22373-22379 · IF 12.732

Self-assembly of a g-C3N4-based 3D aerogel induced by N-modified carbon dots for enhanced photocatalytic hydrogen production

Xiao-Long Pu,Xue-Chun Yang,Shan-Shan Liang,Wenzhong Wang,Jing-Tai Zhao,Zhi-Jun Zhang

An N-modified carbon dots/graphitic carbon nitride (NCDs/g-C3N4) aerogel was successfully prepared by simple electrostatic self-assembly of NCDs and g-C3N4 nanosheets without any harmful solvents or cross-linking agents. The prepared aerogel has a larger specific surface area compared to pure g-C3N4. As the NCD content increased, the NCDs/g-C3N4 aerogel exhibited a wider visible spectral response range and higher photo-generated carrier separation efficiency. It is of note that the hydrogen evolution rate (HER) of the NCDs/g-C3N4 aerogel can reach up to 13 499 μmol h−1 g−1, which is 1.6 times that of pure g-C3N4, because of the advantages of the 3D aerogel structure and the effect of NCDs on photocatalytic activity. The design realizes the control of the morphology of g-C3N4 by NCDs and provides a new strategy for the design of aerogels for highly efficient photocatalysis.

研究领域: 材料科学 · 能源化学 · 环境科学
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POLYMER DEGRADATION AND STABILITY · 2022 · IF 5.204

P, N-decorated halloysite nanotubes for flame retardancy enhancement of polyamide 6/aluminum diethylphosphinate

Wentao He,Huahui Xu,Pingan Song,Yushu Xiang,Shuhao Qin

Flame-retardant functionalized nanomaterials have attracted much research interests due to the combined advantages of organic and inorganic components. In the present study, P, N-decorated halloysite nanotube (MA-PPA@HNT) was prepared via simple steps of phenphosphinic acid intercalation and subsequent electrostatic interaction with melamine. Compared to unmodified HNT, the incorporation of MA-PPA@HNT into polyamide 6 (PA6)/aluminum diethylphosphinic acid (AlPi) composite results in significant improvement of flame retardancy. At equal HNT loading of 2wt%, the UL-94 rating grade of PA6/AlPi/MA-PPA@HNT composite was V-0, whereas that of PA6/AlPi/HNT composite V-2. And compared with PA6 , there is a decrease of peak heat release rate (pHRR) and total heat release (THR) by 72.6% and 17.4%, respectively. The flame retardant mechanism was analyzed by cone calorimetry, gas volatility and characterization of char residues. It is considered that MA-PPA@HNT plays the critical role of promoting the formation of P, Si-rich intumescent char in the condensed phase and enhancing the barrier effect for heat and mass transfer.

CAS / MDL: 108-78-1 701-64-4
研究领域: 材料科学 · 高分子化学
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ACS Catalysis · 2019 · IF 12.221

Photocatalytic Cleavage of Aryl Ether in Modified Lignin to Non-phenolic Aromatics

Hongji Li,Anon Bunrit,Jianmin Lu,Zhuyan Gao,Nengchao Luo,Huifang Liu,Feng Wang

Depolymerization of lignin meets the difficulty in cleaving the robust aryl ether bond. Herein, through installing an internal nucleophile in the β-O-4′ linkage, the selective cleavage of aryl ether was realized by the intramolecular substitution on aryl rings affording non-phenolic arylamine products. In particular, nitrogen-modified lignin models and lignin samples were employed to generate the iminyl radical under photocatalytic reduction, which acted as the internal nucleophile inducing aryl migration from O to the N atom. The following hydrolysis released primary arylamines and α-hydroxy ketones. Mechanism studies including electron spin resonance (ESR), fluorescence quenching experiments, and density functional theory (DFT) calculations proved the aryl migration pathway. This method enables access to non-phenolic arylamine products from lignin conversion.

研究领域: 化学 · 能源 · 环境科学
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CRYSTENGCOMM · 2017 ·Vol. 19 ·期 34 ·4964-4971 · IF 3.474

Synergy of facet control and surface metalloid modification on hierarchical Pt–Ni nanoroses toward high electrocatalytic activity

Qi Zhao,Qin Wang,Yiguo Su,Keke Huang,Guangran Xu,Yingjun Li,Jiayin Liu,Baocang Liu,Jun Zhang

Driven by the need of high catalytic performance and low cost Pt-based catalysts for methanol oxidation (MOR) and oxygen reduction (ORR) reactions, we developed a highly active nitrogen species-decorated Pt–Ni–N catalyst with tunable architectures and facets toward high catalytic activity. The synthetic procedure was conducted by Ni2+-assisted morphology and facet transformation from nanoflowers (NFs) (111) to nanoparticles (NPs) (220) and simultaneous optimization of both hierarchical structure and active surface sites. It is found that the adsorption of nitrogen species plays critical roles in determining both facet control of the Pt–Ni–N hierarchical structure and energetic activation of the catalytic reaction. Decoration of surface nitrogen species can effectually improve the relative content and electronic density of Pt0, leading to formation of a hierarchical structure and significantly improved catalytic activity toward both MOR and ORR compared with Pt–Ni and Pt–N, as well as the commercial Pt/C catalysts, indicating a new strategy to obtain highly efficient catalysts. Moreover, the results demonstrate that the catalytic enhancement is mainly due to the synergistic electronic effects among Pt, Ni, and N species.

研究领域: 材料科学 · 电催化 · 纳米技术
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Millimeter-level nitrogen modified activated carbon spheres assisted Bi4Ti3O12 composites for bifunctional adsorption/photoreduction of CO2

Changming Zhang,Yaqi Wang,Xiaochao Zhang,Rongxian Wang,Lifang Kou,Jiancheng Wang,Rui Li,Caimei Fan

The increase of CO 2 adsorption and separation efficiency of photo-induced carriers are two crucial factors for achieving effective CO 2 reduction into solar fuels. Here, novel millimeter-level nitrogen modified resin-based activated carbon spheres (N-ACSs), as desired support to immobilize and tailor Bi 4 Ti 3 O 12 catalyst (Bi 4 Ti 3 O 12 /N-ACSs) for improving CO 2 photoreduction activities, have been constructed via simple suspension polymerization and impregnation method. The involved TG, FTIR, XRD, XPS, EA, SEM, EDS, N 2 adsorption/desorption, CO 2 adsorption, UV–vis DRS, MS, PC, EIS, PL spectra and in-situ FTIR were characterized. Bi 4 Ti 3 O 12 /N-ACSs displayed the highest photocatalytic CO 2 reduction activity to CO of 142.76 μmol/g under 8 h simulated sunlight irradiation in pure H 2 O phase, approximately 1.45 times and 1.24 times higher than that of pristine Bi 4 Ti 3 O 12 and Bi 4 Ti 3 O 12 /ACSs, respectively. The introduction of N-ACSs played four roles: (i) the increase of CO 2 adsorption, (ii) the red-shift of optical absorption range, (iii) the consummate separation and transfer of photo-induced carriers, (iv) more CO 2 active sites. Finally, the possible mechanism photocatalytic CO 2 reduction for Bi 4 Ti 3 O 12 /N-ACSs was proposed. Our findings should provide noteworthy promising strategy to immobilize powder photocatalyst on the surface of millimeter-level carbon spheres for achieving the high-efficient CO 2 adsorption and photoreduction to CO.

CAS / MDL: 108-39-4
研究领域: 材料科学 · 环境科学 · 能源科学
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ACS Catalysis · 2019 · IF 12.221

Visible-Light-Driven Selective Oxidation of Toluene into Benzaldehyde over Nitrogen-Modified Nb2O5 Nanomeshes

Kaiyi Su,Huifang Liu,Bin Zeng,Zhixin Zhang,Nengchao Luo,Zhipeng Huang,Zhuyan Gao,Feng Wang

Photocatalytic selective oxidation of hydrocarbons to oxygenated chemicals greatly relies on catalytic materials that show high efficiency of photogenerated holes and electrons separation and visible light absorption capacity. We, herein, report one facile calcination approach with ammonium chloride and melamine as the template to synthesize nitrogen-modified Nb2O5 nanomeshes material (Nb2O5-N), which exhibits a 37-fold reaction rate larger than its commercial counterpart in photocatalytic oxidation of toluene into benzaldehyde under visible light irradiation. The reactivity is ascribed to an extended absorption spectrum within 700 nm by nitrogen modification. In addition, photocurrent response results suggest that a relaxation effect induced by nanomesh structure is beneficial for the separation of charge carriers for enhanced reactivity. This work sheds light on regulating the structure of metal oxides and the application of nanomesh materials in photocatalytic hydrocarbon conversion.

CAS / MDL: 122-00-9 108-78-1
研究领域: 材料科学 · 化学工程 · 环境科学
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 10 ·5416-5425 · IF 10.733

Surface nitrogen-modified 2D titanium carbide (MXene) with high energy density for aqueous supercapacitor applications

Yapeng Tian,Wenxiu Que,Yangyang Luo,Chenhui Yang,Xingtian Yin,Ling Bing Kong

Supercapacitors (SCs), environment-friendly high-power energy storage devices, have drawn great attention due to the increasing and urgent development of renewable energies. Ti3C2Tx (MXene), a 2D high conductivity material, has been shown to be a potential electrode material for SCs, because of its outstanding chemical and physical properties. However, the surface termination of –F and –OH could block the transport of electrolyte ions and thus decrease the energy storage performances. In this regard, nitrogen related functional groups have been introduced to modify the surface characteristics of Ti3C2Tx, in order to increase the electron conduction and energy storage capacity. Experimental results have shown that the presence of moieties such as –NH2, Ti–O–N and O–Ti–N, could offer a synergistic effect on the electrochemical performance of SCs, which is mainly attributed to the intercalation-pseudocapacitance contribution according to the quantitative analysis. Furthermore, the role of O–Ti–N is more significant than that of Ti–O–N. Specifically, for the first time, we demonstrate that electrodes based on the N surface modified Ti3C2Tx film display largely enhanced electrochemical performances, with gravimetric capacitance of 415.0 F g−1 at 2 mV s−1, rate capacity of 75.9% at 200 mV s−1 and cycling stability of above 90% retention after 18 000 cycles. In addition, symmetric SCs based on the N–Ti3C2Tx-300 film could deliver a maximum volumetric energy density of 21.0 W h L−1 and an energy density of 10.2 W h L−1, at a high power density of 18.3 kW L−1.

研究领域: 材料科学 · 能源存储技术
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Porous TiN-based ceramic electrode with N-modified Co-based Nanorods/TiN heterointerfaces for efficient overall water splitting

Chuntian Tan,Haisen Huang,Feihong Wang,Nianwang Ke,Anding Huang,Wangzhong Tang,Luyuan Hao,Liangjun Yin,Xin Xu,Yuxi Xian,Simeon Agathopoulos

The development of high-performance electrocatalytic electrodes for overall water splitting is a crucial issue to realize renewable hydrogen production . This paper presents the in situ growth of N -modified Co-based nanorods on porous TiN ceramic membranes using the hydrothermal method and thermal NH 3 treatment, resulting in a novel self-supported electrocatalytic electrode with abundant heterointerfaces, denoted as NCTN-x-y (x: nitridation temperature; y: nitridation time). In the alkaline medium (1 M KOH), the NCTN-350-2 electrode displays the best hydrogen evolution reaction (HER) activity (ƞ 10  = 66 mV), and the NCTN-250-3 electrode manifests the best oxygen evolution reaction (OER) performance (ƞ 10  = 270 mV). Accordingly, these two electrodes comprise an electrolyzer, which features a current density of 10 mA cm −2 at a low cell voltage of 1.63 V. The good electrocatalytic performance can be attributed to the abundant heterointerfaces formed between the porous TiN ceramic membrane and the N -modified Co-based nanorods , in conjunction with the hierarchical pore structure of the TiN ceramic membrane. Theoretical calculations identify that the construction of heterointerfaces modulates the electronic structure of active sites, thereby promoting the dissociation of H 2 O, optimizing the H* adsorption energy (ΔG H* ), and accelerating the reaction kinetics, which ultimately improve the electrocatalytic activity of electrode.

CAS / MDL: 12036-10-1 25583-20-4
研究领域: 材料科学 · 电化学 · 可再生能源
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BIOPROCESS AND BIOSYSTEMS ENGINEERING · 2023 · IF 3.8

Enhancing diversified extracellular electron transfer (EET) processes through N-MXene-modified non-adhesive hydrogel bioanodes

Zhong Linhan,Chen Ye,Wen Qing,Yang Yang

The focus of this study is to develop a high-performance anode material for microbial fuel cells (MFCs). PEDOT:PSS and nitrogen-modified MXene were combined to create a hydrogel composite material called PPNM, which was drop-cast onto carbon felt (CF) as the MFCs anode. The PPNM exhibited a higher peak power density of 4.78 W m −2 , an increase of 332% compared to the CF anode. It is worth noting that the PPNM Hydrogel maintains its rough and porous structure, providing favorable sites for bacterial colonization. The introduction of N-MXene has improved the electrochemical performance of the hydrogel, particularly impacting the mediated electron transfer process. Microbial community analysis revealed the presence of more electrochemically active species on the PPNM anode. These findings highlight the potential of PPNM hydrogel and pave the way for similar strategies in achieving high-performance anodes in MFCs.

研究领域: 生物工程 · 材料科学 · 环境微生物学
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ANALYST · 2025 ·Vol. 150 ·期 4 ·650-660 · IF 3.3

Nitrogen-modified reduced graphene oxide for serum enrichment of N-glycans and MALDI-TOF MS-based identification of HCC biomarkers

Baoying Zhang,Shengjie Yang,Xuyuan Chao,Lu Qi,Weijie Qin,Haihong Bai,Xinghe Wang

Protein N-glycosylation, as one of the most crucial post-translational modifications, plays a significant role in various biological processes. The structural alterations of N-glycans are closely associated with the onset and progression of numerous diseases. Therefore, the precise and specific identification of disease-related N-glycans in complex biological samples is invaluable for understanding their involvement in physiological and pathological processes, as well as for discovering clinical diagnostic biomarkers. However, protein N-glycosylation suffers from microscopic heterogeneity and low abundance in biological systems, leading to N-glycopeptide signals being overshadowed by those of their non-glycosylated counterparts during mass spectrometry (MS) analysis. Consequently, there is an urgent demand for the development of novel methods for highly efficient N-glycan enrichment. In this study, we introduced a novel hydrophilic nanomaterial, nitrogen-modified reduced graphene oxide (N-rGO), tailored for this purpose, which was formed by a condensation reaction between the amino groups of rGO and the carboxyl groups of Fmoc-Photo-Linker. Compared to other enrichment materials, N-rGO not only supports efficient N-glycans enrichment via hydrophilic interaction (HILIC), but also serves as an effective matrix for direct MALDI-TOF MS analysis combined with DHB, thereby avoiding sample loss during N-glycans release. 76 and 81 serum N-glycans were obtained from 3 healthy individuals and 3 hepatocellular carcinoma (HCC) patients. Notably, relative quantification of serum N-glycans between 20 patients and 20 healthy controls showed significant expression differences, such as H5N4F1S1, H6N5F1, H5N4S2, H5N4F2S1 and H5N5F1S1, indicating the potential of N-rGO for biomarker discovery.

研究领域: 生物化学 · 医学诊断 · 分子生物学
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