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AICHE JOURNAL · 2021 ·Vol. 67 ·期 6 ·e17197 · IF 3.993

Quasi-continuous synthesis of iron single atom catalysts via a microcapsule pyrolysis strategy

Liyun Huang,Kui Wu,Qian He,Chao Xiong,Tao Gan,Xiaohui He,Hongbing Ji

Single atom catalysts (SACs), featured with atomically dispersed metal species, have been considered as one of the most promising catalytic materials because of the excellent performance in various high-value-added reactions. However, the large-scale and continuous-type production of such SACs is still challenging. Herein, a novel and facile microcapsule strategy for the quasi-continuous synthesis of iron SACs supported on S, N co-doped carbon (Fe/SNC) is developed, and the Fe species are presented as isolated active sites and stabilized as the FeN 3 S-like structure. The as-prepared Fe/SNC catalysts exhibit excellent catalytic properties for selective oxidation of arylalkanes, which followed pseudo-first-order kinetics with an E a = 41.5 kJ/mol. More importantly, the two Fe/SNC catalysts synthesized at different continuous times showed essentially identical catalyst structure and catalytic performance, demonstrating the superior reliability of our microcapsule strategy for the quasi-continuous production of SACs, which can be easily scaled up to industrial application.

研究领域: 催化化学 · 材料科学
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Journal of Materials Chemistry A · 2024 · IF 10.7

Interfacial modulation of Ru catalysts using B, N co-doped porous carbon-confined MoC quantum dots for enhanced hydrogen evolution reaction performance

Shumin Xie,Mang Niu,Xingyun Li,Yang Lei,Huanfang Zhang,Shuai Xu,Deyu Wang,Sameh M. Osman,Zhi Peng,Yusuke Yamauchi

The development of high-performance electrocatalysts that rival Pt catalysts is crucial for efficiently driving the hydrogen evolution reaction (HER) to produce H2. Herein, we engineer sophisticated interfacial modulation of the Ru catalysts by constructing B, N co-doped porous carbon confined ultra-small MoC quantum dots (MoC@BNC) as an advanced catalyst carrier and stimulator. Combined experimental and theoretical calculations prove enhanced electron interaction between the Ru catalysts and the MoC quantum dots. Additionally, the B, N co-doped carbon substrate further refines the electronic structure of MoC, reinforcing the modulation of Ru catalysts. The Ru/MoC@BNC catalyst embodies a boosted H2O dissociation ability with a lowered H bonding strength, which promises an outstanding HER performance with an overpotential of 14 mV at 10 mA cm−2 in an alkaline solvent. Furthermore, robust catalytic stability is achieved with almost zero deterioration after the cycling test. This result exemplifies the importance of interfacial manipulation of the Ru catalysts to promote HER catalytic performance.

CAS / MDL: 10043-35-3
研究领域: 材料科学 · 催化化学 · 能源科学
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JOURNAL OF NANOPARTICLE RESEARCH · 2023 ·Vol. 25 ·期 8 ·1-10 · IF 2.5

Fast degradation of rhodamine B by peroxymonosulfate activated with Fe–N carbon nanotubes

Cui Wei,Fang Jiahui,Wan Yuanyuan,Tao Xueyu,Guo Litong,Feng Qiyan

In this study, Fe–N co-doped carbon nanotubes (Fe–N-CNTs) were prepared and used to activate peroxymonosulfate (PMS) for advanced oxidation removal of Rhodamine B (RhB). The XRD, XPS, SEM and EDS results revealed that the Fe, N, O co-doped carbon nanotubes (Fe–N-CNTS) coated with FeO(OH) nanosheets were successfully synthesized by a simple pyrolyzing process. The large BET specific surface area (286.42 m 2 /g) and hybrid pore structure of micropores and mesopores (3–10 nm) of the Fe–N-CNTS ensured its good RhB degradation performance (98% in 30 min) by activatting PMS. The Fe–N-CNTS-1.5 had the best degradation performance, which could be attributed to the synergy effect between FeO(OH) nanosheets and Fe–N-CNTS. The 1 O 2 , O 2 •, •OH and SO 4 −• were formed during the PMS activating process and involved in the RhB degradation. The reaction constant of 0.5483 min −1 could be obtained by adding 1.5 mM PMS, which is about 12 and 24 times of the reaction constant of PMS only (0.0458 min −1 ) and FeN-CNTS only (0.0226 min −1 ), respectively. This work provides new insight into the mechanism of PMS activation by carbon-based catalysts for the efficient degradation of RhB.

研究领域: 环境科学 · 材料科学
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OPTICAL MATERIALS · 2021 · IF 3.08

Alkali-assisted synthesis of gourd flesh derived tricolor F/N co-doped carbon dots for efficient degradation of organic dyes

Congling Wang,Jun Xu,Huizhi Li,Weilin Zhao

A novel tricolor F/N co-doped CDs was synthesized by alkali-assisted control with gourd flesh as a precursor, targeting at the catalytic degradation of organic dyes with extremely high catalysis rate. The synthesized nanomaterials were characterized by X-ray diffraction, Transmission electron microscopy , Fourier transform infrared spectra and X-ray photoelectron spectroscopy techniques, indicating that the tricolor F/N-CDs have good dispersion and abundant surface defects which were gradually increasing from F/N-G-CDs, F/N-Y-CDs to F/N- O -CDs. Through the UV–visible and fluorescence spectra , the tricolor F/N-CDs all exhibited good fluorescence performance and the fluorescence lifetime was nano-scale level. The tricolor F/N-CDs displayed excellent photocatalytic activity which was evaluated by the organic dyes methylene blue (MB) and congo red (CR) as models. The important thing is that under sunlight irradiation, the degradation efficiency of using tricolor F/N-CDs for MB reaches ~100% and the degradation efficiency for CR dye reaches ~98% in a pole short time. With the red shift of the fluorescent tricolor F/N-CDs, the degradation time gradually decreased and the degradation rate gradually increased. The results explained that the prepared tricolor F/N-CDs had excellent application prospects in the natural degradation.

CAS / MDL: 1310-73-2
研究领域: 材料科学 · 环境科学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2021 · IF 5.316

Heterogeneous Co@CoO composited P, N co-doped carbon nanofibers on carbon cloth as pH-tolerant electrocatalyst for efficient oxygen evolution

Xiaoming Fan,Yuyin Fan,Xiao Zhang,Lin Tang,Jinxue Guo

Heterostructured materials favoring synergism, efficient charge transfer, and abundant active sites have aroused enormous interests for water electrolysis. Here heterogeneous Co@CoO encapsulated in P, N co-doped carbon nanofibers supported on carbon cloth (Co@CoO-PNC/CC) has been prepared to pursue attractive synergism for the application of pH-tolerant catalyst for oxygen evolution reaction (OER) in both alkaline and neutral solutions. The prepared Co@CoO-PNC/CC exhibits advanced OER performances, generating a current density of 10 mA cm −2 at overpotential of 289 mV in alkaline media and 371 mV in neutral media. The high OER activity can be assigned to the synergistic effect of abundant active sites and enhanced charge transfer between Co and CoO, as well as the specific P, N co-doped carbon nanofiber architecture.

研究领域: 材料科学 · 电化学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2023 · IF 4.4

Transfer, transportation, and adsorption of UV-B by Mg-N co doped carbon quantum dots: Response of growth indicators, antioxidant effect and mechanism explanation

Yu Zhang,Ying Huang,Junhong Jiang,Jianbo Chen,Weixing Han,Yuxian Liu,Linjun Kong,Jian Gong,Minhua Su,Diyun Chen

Mg and N co-doped carbon quantum dots (Mg-N-CQDs) were synthesized and applied to alleviate oxygen toxicity by UV-B radiation and enhance antioxidative responses to wheat seedlings. It showed that Mg-N-CQDs pre-treatment attenuated the UV-B stress effects in a dose-dependent manner, as indicated by enhancing the characteristics of seed germination and early seedling growth parameters. Meanwhile, Mg-N-CQDs can be applied in plant nutrient solutions with nitrogen, phosphorus, potassium, and other fertilizers to promote the growth of seedlings. Furthermore, efficient antioxidant systems, chlorophyll content, and stability of fluorescence intensity were activated by Mg-N-CQDs pre-treatment, which effectively increased the activities of superoxide dismutase (SOD), catalase (CAT), and peroxidase (POD), and eliminate the contents of malondialdehyde (MDA) and hydrogen peroxide, and the production rate of superoxide anion radical in the roots and germs, thereby preventing oxidative damage from UV-B stress. Notably, Mg-N-CQDs pre-treatment significantly increased the expression of related genes to improve the antioxidant capacity of roots and germs, resulting in an increased level of ATPS, CS, and GS. The mechanism study indicated that amino and hydroxyl groups and Mg, N modified CQDs could broaden the light absorption range of CQDs and improve the ability to convert blue light and ultraviolet rays to visible light, which was the main reason why Mg-N-CQDs could relieve wheat seedlings from ultraviolet stress. Therefore, Mg-N-CQDs could serve as a regulator to reduce the damage of UV-B, laying the foundation for their application in environmental protection and agricultural production.

研究领域: 植物学 · 环境科学 · 农业科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Ultrafine palladium nanoparticles deposited on Ni, N co-doped carbon to boost dehydrogenation efficiency of perhydro-N-phenylcarbazole

Linsen Li,Zhuwei Yang,Xiao Yang,Hui Xiong,Zhao Jiang,Tao Fang

Liquid organic hydrogen carriers (LOHCs) are considered as promising candidates for large-scale hydrogen storage, which offers significant advantages in terms of hydrogen storage density, ease of storage and transportation. NPhCZ (N-phenylcarbazole)/18H-NPhCZ (perhydro-N-phenylcarbazole) is proposed as a typical system with high hydrogen storage capacity. However, low dehydrogenation activity and selectivity of catalysts restrict the cyclic efficiency of hydrogen storage. In this study, the efficient catalysts are designed by the immobilization of ultrafine, highly dispersed Pd nanoparticles onto Ni, N co-doped carbon materials through wet chemical reduction. The Pd/Ni@NC-10 catalyst exhibits the highest catalytic performance with 100 % conversion, 81.9 % selectivity of NPhCZ and 6.48 wt% hydrogen release amount. Combined with XRD, HRTEM, Raman, XPS, H 2 -TPR, N 2 physisorption characterization methods and DFT calculations, it is found that the doped Ni, N species could synergistically increase the dispersion of loaded Pd nanoparticles, as well as regulate the electronic state around Pd, which in turn accelerates the rate of the rate-limiting step. The evident interaction between Pd nanoparticles and Ni, N co-doped carbon brings the enhancement of dehydrogenation efficiency. Besides, the spent catalysts are measured by XRD, TEM, XPS and evaluated for the dehydrogenation reaction, indicating that Pd/Ni@NC-10 shows good structural stability, durability and recyclability. It provides practical guidance for the design of LOHCs dehydrogenation catalysts.

研究领域: 材料科学 · 催化化学
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Journal of Physical Chemistry C · 2024 · IF 3.3

High Efficiency Degradation Organic Pollutant Using Novel Heme-Derived Fe–N Co-Doped Carbon Catalyst Activated PDS and H2O2

Caiyi Jiang,Ming Hou,Li Yang,Shenghui Guo,Guo Yang,Bo Xing,Yi Wang,Dongzheng Wang,Xiaolin Shi

Fe–N co-doped carbon catalyst has received increasing attention in the field of organic wastewater treatment because of its unique structure and outstanding activity. However, the reusability, catalytic activity, and pH working range are still a great challenge for future application. Herein, a novel αFe-HM@C-T catalyst was prepared by pyrolyzing a mixture of starch and heme and was analyzed by TEM, H2-TPR, XRD, BET, XPS, FTIR, and Raman spectrum. Meanwhile, αFe-HM@C-T catalysts show the highest catalytic performance due to abundant porous structure, higher redox property, and unique Fe–Nx configuration. The rhodamine B (RhB) could be almost completely degraded within 30 min on the 5Fe-HM@C-850, and recovery rates of catalytic activity of 96% and 91.8% were achieved in peroxydisulfate (PDS) and H2O2 systems with an extensive buffer pH range. Furthermore, mechanistic insights by quenching experiments and EPR verified the high removal efficiency of RhB mainly attributed to indirect oxidation of SO4•–, •OH, and 1O2 in both systems, and the potential mechanism was proposed.

研究领域: 环境科学 · 催化材料科学
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Journal of Energy Chemistry · 2020 · IF 7.216

Wavelength-sensitive photocatalytic H2 evolution from H2S splitting over g-C3N4 with S,N-codoped carbon dots as the photosensitizer

Zhanghui Xie,Shan Yu,Xiang-Bing Fan,Shiqian Wei,Limei Yu,Yunqian Zhong,Xue-Wang Gao,Fan Wu,Ying Zhou

Photocatalytic splitting of hydrogen sulfide (H 2 S) for hydrogen evolution is a promising method to solve the energy and environmental issues. In this work, S,N-codoped carbon dots (S,N-CDs)/graphitic carbon nitride (g-C 3 N 4 ) nanosheet is synthesized by hydrothermal method as an efficient photocatalyst for the decomposition of H 2 S. In addition to the characterization of the morphology and structure, chemical state, optical and electrochemical performances of S,N-CDs/g-C 3 N 4 , hydrogen evolution tests show that the activity of g-C 3 N 4 is improved by introducing S,N-CDs, and the enhancement depends strongly on the wavelength of incident light. The photocatalytic hydrogen production rate of S,N-CDs/g-C 3 N 4 composite reaches 832 μmol g −1 h −1 , which is 38 times to that of g-C 3 N 4 under irradiation at 460 nm. Density functional theory calculations and electron paramagnetic resonance as well as photoluminescence technologies have altogether authenticated that the unique wavelength-dependent photosensitization of S,N-CDs on g-C 3 N 4 ; meanwhile, a good match between the energy level of S,N-CDs and g-C 3 N 4 is pivotal for the effective photocatalytic activity. Our work has unveiled the detailed mechanism of the photocatalytic activity enhancement in S,N-CDs/g-C 3 N 4 composite and showed its potential in photocatalytic splitting of H 2 S for hydrogen evolution.

CAS / MDL: 68-12-2
研究领域: 材料科学 · 环境科学 · 化学
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LUMINESCENCE · 2016 ·Vol. 32 ·期 3 ·277-284 · IF 1.452

Highly luminescent S,N co-doped carbon quantum dots-sensitized chemiluminescence on luminol–H2O2 system for the determination of ranitidine

Jianqiu Chen,Juan Shu,Jiao Chen,Zhiran Cao,An Xiao,Zhengyu Yan

S,N co-doped carbon quantum dots (N,S-CQDs) with super high quantum yield (79%) were prepared by the hydrothermal method and characterized by transmission electron microscopy, photoluminescence, UV–Vis spectroscopy and Fourier transformed infrared spectroscopy. N,S-CQDs can enhance the chemiluminescence intensity of a luminol–H 2 O 2 system. The possible mechanism of the luminol–H 2 O 2 –(N,S-CQDs) was illustrated by using chemiluminescence, photoluminescence and ultraviolet analysis. Ranitidine can quench the chemiluminescence intensity of a luminol–H 2 O 2 –N,S-CQDs system. So, a novel flow-injection chemiluminescence method was designed to determine ranitidine within a linear range of 0.5–50 μg ml −1 and a detection limit of 0.12 μg ml −1 . The method shows promising application prospects.

CAS / MDL: 521-31-3
研究领域: 分析化学 · 药物分析
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Precise electronically modulated Mn doped nickel iron phosphate with P, N codoped carbon decorated P-doped carbonized bacterial cellulose for efficient electrocatalytic glucose conversion coupled with H2 generation

Ning Wei,Sufeng Zhang,Xue Yao,Yao Feng,Valentin Nica,Jinfan Yang,Qiusheng Zhou

Biomass electrocatalytic-conversion coupled with hydrogen generation exhibits low energy consumption, efficient hydrogen production and green syntheses of value-added chemicals. However, constructing electrocatalysts with precise electronic modulation and structures for efficient biomass electrocatalytic conversion coupled hydrogen production remains challenging. Herein, a bacterial cellulose substrate was combined in situ with a Mn-doped NiFe Prussian blue analogue (PBA) precursor, and one-step carbonization-phosphorylation was developed for the preparation of Mn-doped nickel iron phosphate (MNFP) embedded in a P, N codoped carbon (PNC) substrate grown directly on P-doped carbonized bacterial cellulose (MNFP-PNC/PCBC). Benefiting from the three-dimensional network structure of P-doped carbonized bacterial cellulose (PCBC) and atomic doping, MNFP-PNC/PCBC exhibited an optimized electronic structure, abundant active sites and excellent electrical conductivity. Therefore, the voltages required with hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and glucose electrocatalytic-conversion (GCR) to drive a current density of 50 mA cm −2 were 0.214, 1.5, and 1.34 V, respectively. Moreover, the required cell voltage of the novel electrolyser containing MNFP-PNC/PCBC as electrodes can be further reduced to 1.55 V at 50 mA cm −2 compared to overall water splitting, resulting in more than 8-time improvement in hydrogen production efficiency and production of value-added formate. This work provides a unique approach for electrocatalytic-conversion of biomass coupled with electrocatalytic hydrogen generation.

研究领域: 材料科学 · 电化学 · 能源转换
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Peapod-Like Structured B/N Co-Doped Carbon Nanotube Array Encapsulating MxPy (M = Fe, Co, and Ni) Nanoparticles for High-Rate Potassium Storage

Xiwen Tao,Zhengguang Zhang,Zheng Li,Shuangsheng Xiong,Shengmei Wang,Faming Gao,Chen Wang,Li Hou

Potassium-ion batteries (PIBs) have become the desirable alternatives for lithium-ion batteries (LIBs) originating from abundant reserves and appropriate redox potential, while the considerable radius size of K+ leading to poor reaction kinetics and huge volume expansion limits the practical application of PIBs. Hybridization of transition-metal phosphides and carbon substrates can effectively optimize the obstacles of poor conductivity, sluggish kinetics, and huge volume variation. Thus, the peapod-like structural MxPy@BNCNTs (M = Fe, Co, and Ni) composites as anode materials for PIBs were synthesized through a facile strategy. Notably, the unique architecture of B/N codoped carbon nanotube array as fast ion/electron transfer pathways effectively improves the electronic conductivity of composites. The MxPy nanoparticles (NPs) are encapsulated in BNCNTs with an amorphous carbon layer (5–10 nm), which discernibly alleviate the volume changes during potassiation/depotassiation. In conclusion, the composites show a commendable cycling performance, possessing reversible capacities of 111, 152, and 122 mA h g–1 after 1000 cycles at 1.0 A g–1 with a negligible capacity loss for FeP@BNCNT, CoP/Co2P@BNCNT, and Ni2P@BNCNT electrodes, respectively. Especially, after 1000 cycles at 2.0 A g–1, the CoP/Co2P@BNCNT electrode still possesses a capacity of 87.9 mA h g–1, demonstrating excellent rate performance and long-term life. This work may offer an innovative and viable route to construct a stable architecture for solving the issue of poor stability of TMP-based anodes at a high current density.

研究领域: 材料科学 · 能源存储
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