APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Feng Du,Zhikun Yao,Jikai Xiang,Jingsha Li,Changhong Wang,Chunmei Zhang,Tao Hu,Jinlong Liu,Changming Li,Chunxian Guo
To design high-performance electrocatalysts with desired electronic structures is critical to facilitate the conversion of pollutant nitrate (NO 3 − ) to value-added ammonia (NH 3 ) at ambient condition. Nevertheless, the current electrocatalysts for NO 3 − -to-NH 3 still face low Faradaic efficiency and selectivity. We present here a heteroatoms co-doped strategy using phosphorus (P) and oxygen (O) to tune electronic structure of copper (Cu) nanocrystals to form highly active surface for selective NO 3 − -to-NH 3 . By combing experimental results and theoretical calculation, it is found that the heteroatom P, O-doping can negatively shift the Cu d -band center, which optimizes adsorption energies of intermediates, especially for *NO 3 − and *NH 3 . The P, O-doped Cu nanocrystal exhibits an efficient 8-electron transfer process for NO 3 − -to-NH 3 . It achieves both high NO 3 − conversion rate (91.09 %) and NH 3 Faradaic efficiency (91.72 %) in high concentration NO 3 − electrolyte (1.0 M KOH + 1400 ppm NO 3 − -N), retaining its potential applications in practical NO 3 − -to-NH 3 .
研究领域:
材料科学
·
电催化
·
环境科学
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 2
·e7980
·
IF 0
Yong Yang,Wei He,Dengmeng Song,Fang Xie,Jiaying Li,Jun Li,Ning Wang
A D-A 1 -A 2 type covalent triazine framework (CTF) was prepared for the photocatalytic hydrogen evolution (HER). In the resulting CTF-CZ-Bpy 2+ , 9-ethyl-9 H -carbazole (CZ) group is used as the donor, triazine ring as the first acceptor, and cyclic diquat (Bpy 2+ ) moiety as the second acceptor. Both experimental and theoretical results show that the D-A 1 -A 2 structure significantly enhances the efficiency of photogenerated charge separation and transfer. As a result, CTF-CZ-Bpy 2+ demonstrated outstanding photocatalytic HER activity with a yield rate of 31.1 mmol g −1 h −1 , which is 7.8 times higher than that of nonfunctionalized CTF-CZ-Bpy.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
SYNTHETIC METALS
·
2013
·
IF 2.109
Wang Gang,Tan Haijun,Zhang Yiping,Wu Yingying,Hu Zhubin,Yu Guipeng,Pan Chunyue
Novel D-π-A system organic dyes (ID1, ID2 and ID3) based on isoindigo (ID), which contain triphenylamine (ID1) or isoindigo (ID2 and ID3) as electron donors, isoindigo and thiophene as a π-conjugated system and a cyanoacrylic acid moiety as an electron acceptor and anchoring group, have been then synthesized and characterized by 1 H NMR, UV–vis, CV. Dye-sensitized solar cells (DSSCs) based on these dyes were also fabricated and tested. As the photovoltaic performance tests demonstrated, the ID1 exhibits broader absorption spectra , higher maximum incident photon-to-current conversion efficiency (IPCE) and maximum photon-to-electron conversion efficiency ( η ) of 3.33% under 100 mW/cm 2 simulated AM 1.5G solar irradiation.
研究领域:
材料科学
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能源科学
·
有机化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Yaqi Li,Sijie Wan,Weichen Liang,Bei Cheng,Wang Wang,Yao Xiang,Jiaguo Yu,Shaowen Cao
Owing to the improved charge separation and maximized redox capability of the system, Step-scheme (S-scheme) heterojunctions have garnered significant research attention for efficient photocatalysis of H 2 evolution. In this work, an innovative linear donor–acceptor (D–A) conjugated polymer fluorene-alt-(benzo-thiophene-dione) (PFBTD) is coupled with the CdS nanosheets, forming the organic–inorganic S-scheme heterojunction. The CdS/PFBTD (CP) composite exhibits an impressed hydrogen production rate of 7.62 mmol g −1 h −1 without any co-catalysts, which is ≈14 times higher than pristine CdS. It is revealed that the outstanding photocatalytic performance is attributed to the formation of rapid electron transfer channels through the interfacial Cd─O bonding as evidenced by the density functional theory (DFT) calculations and in situ X-ray photoelectron spectroscopy (XPS) analysis. The charge transfer mechanism involved in S-scheme heterojunctions is further investigated through the photo-irradiated Kelvin probe force microscopy (KPFM) analysis. This work provides a new point of view on the mechanism of interfacial charge transfer and points out the direction of designing superior organic–inorganic S-scheme heterojunction photocatalysts.
研究领域:
材料科学
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化学工程
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光化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Xiaofeng Wang,Xiao Liu,Lixue Wu,Gang Hu,Zhaohui Fang
Chiral enantiomers of drugs often exhibit distinct pharmacological activities despite their similar physical and chemical properties. Developing efficient methods for their distinguishment is crucial for pharmaceutical quality control. Here, we presented a novel approach using a CTT (Chlorite-Tetramethylammonium Hydroxide-Tetrathionate) clock reaction system for kinetic chiral enantiomer recognition. DOPA enantiomers were selected for this purpose, in which L-DOPA is therapeutic efficacy in treating Parkinson's disease by precursoring dopamine while D-DOPA lacks such a function. By introducing equal amounts of L-DOPA and D-DOPA into the CTT clock system, we observed a more prolonged induction period for L-DOPA compared to D-DOPA, enabling their quick differentiation. Moreover, a linear relationship between the induction period and the concentration (1.190 × 10 −6 mol/L to 4.5238 × 10 −6 mol/L) of L-DOPA or D-DOPA allowed quantitative detection of L-DOPA or D-DOPA samples. This method could also be applied to analyze varying concentration ratios of L-DOPA and D-DOPA mixtures at a fixed total concentration. Study on mechanism indicates that both L-DOPA and D-DOPA react with ClO 2 · radical to finally generate DHICA through oxidation, with their kinetic disparities evident during this process. These kinetic disparities between L-DOPA and D-DOPA oxidation arises from stereospecific hydrogen-bonding interactions in the cyclodopa intermediate. The weaker hydrogen bond in L-DOPA-derived cyclodopa likely facilitates its cleavage during oxidation, thereby accounting for the faster reaction kinetics observed in the clock system compared to D-DOPA. This makes L-DOPA exhibit more fast consumption of chlorine dioxide than D-DOPA, and resulting larger the extension in the induction period with L-DOPA than that with D-DOPA. Such a method coupling CCT clock demonstrates its versatility and potential for broader applications in chiral drug analysis.
研究领域:
分析化学
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手性药物分析
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药学
·
化学动力学
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 47
·37574-37580
·
IF 3.84
Chao-Feng Du,Lei Jiang,Lei Sun,Nian-Yu Huang,Wei-Qiao Deng
We synthesized a D–π–A–π–A type dye and demonstrated its application in dye-sensitized solar cells (DSSCs). This D–π–A–π–A type dye, named C321, consisted of a triphenylamine as a donor, a 3,4-ethylenedioxythiophene (EDOT) as a π-bridge, and a benzothiazole (BTDA)–phenyl-cyanoacrylic acid as an A–π–A group. Compared with DSSCs based on a traditional D–π–A type dye C311, the DSSCs based on C321 exhibited a significant enhancement of cell performance. A power conversion efficiency of 8.2% was achieved for DSSCs based on C321, which was 9 times higher than that for DSSCs based on C311 (0.9%). The theoretical calculations and electrochemical impedance spectroscopy investigations revealed the mechanism of the enhancement of cell performance.
研究领域:
材料科学
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能源技术
·
有机化学
✓ 已验证
DOI
高影响因子
Small
·
2024
·
IF 13
Min Yan,Ranran Wei,Ruifan Zhang,Xiaoying Zhang,Shiqin Sun,Xuewen Wei,Xianlong Wang,Shuli Yin,Yinglong Wang
Electrochemical nitrite reduction reaction ( NO 2 − RR ${\mathrm{NO}}_{\mathrm{2}}^{\mathrm{ - }}{\mathrm{RR}}$ ), as a green and sustainable ammonia synthesis technology, has broad application prospects and environmental friendliness. Herein, an unconventional p - d orbital hybridization strategy is reported to realize the fabrication of defect-rich CuSb porous nanonetwork (CuSb PNs) electrocatalyst for NO 2 − RR ${\mathrm{NO}}_{\mathrm{2}}^ - {\mathrm{RR}}$ . The crystalline/amorphous heterophase structure is cleverly introduced into the porous nanonetworks, and this defect-rich structure exposes more atoms and activated boundaries. CuSb PNs exhibit a large NH 3 yield ( r N H 3 ${{r}_{{\mathrm{N}}{{{\mathrm{H}}}_{\mathrm{3}}}}}$ ) of 946.1 µg h −1 m cat − 1 ${\mathrm{m}}_{{\mathrm{cat}}}^{ - {\mathrm{1}}}$ and a high faradaic efficiency (FE) of 90.7%. Experimental and theoretical studies indicate that the excellent performance of CuSb PNs results from the defect-rich porous nanonetworks structure and the p-d hybridization of Cu and Sb elements. This work describes a powerful pathway for the fabrication of p - d orbital hybrid defect-rich porous nanonetworks catalysts, and provides hope for solving the problem of nitrogen oxide pollution in the field of environment and energy.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Dandan Zhu,Meijuan Chen,Yu Huang,Rong Li,Tingting Huang,Jun-ji Cao,Zhenxing Shen,Shun Cheng Lee
Formaldehyde is a typical indoor air pollutant that has posed severely adverse effects on human health. Herein, a novel FeCo alloy nanoparticle-embedded nitrogen-doped carbon (FeCo@NC) was synthesized with the aim of tailoring the transition-metal d-band structure toward an improved formaldehyde oxidation activity for the first time. A unique core@shell metal–organic frameworks (MOFs) architecture with a Fe-based Prussian blue analogue core and Co-containing zeolite imidazole framework shell was firstly fabricated. Then, Fe and Co ion alloying was readily achieved owing to the inherent MOF porosity and interionic nonequilibrium diffusion occurring during pyrolysis . High-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectra confirm that small FeCo alloys in situ form in FeCo@NC, which exhibits a higher formaldehyde removal efficiency (93%) than the monometallic Fe-based catalyst and a remarkable CO 2 selectivity (85%) at room temperature. Density functional theory calculations indicate the number of electrons transferred from the metal core to the outer carbon layer is altered by alloying Fe and Co. More importantly, a downshift in the d-band center relative to the Fermi level occurs from − 0.93 to − 1.04 eV after introducing Co, which could alleviate the adsorption of reaction intermediates and greatly improve the catalytic performance.
研究领域:
环境科学
·
材料科学
·
化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 86
·70139-70146
·
IF 3.84
Xing-Long Li,Tao Pan,Jin Deng,Yao Fu,Hua-Jian Xu
Furfural is a biomass-based bulk chemical and its derivatives have potential applications as renewable fuels and chemicals. A water-tolerant and stable solid acid catalyst modified hydrated tantalum oxide (TA-p) was developed for catalytic conversion of D-xylose to furfural in water–organic solvent biphasic system. This process was performed both in a batch reactor and a continuous fixed-bed reactor. In the batch process, D-xylose conversion and furfural yield were significantly affected by the organic solvent, reaction temperature and reaction time. 1-Butanol, which could be obtained through the fermentation of biomass-based carbohydrates, was selected as organic phase and the highest furfural yield of 59% was achieved with D-xylose conversion of 96% at 180 °C in the continuous process. Moreover, the long-time stability test for 80 h under the optimal conditions showed the excellent stability of TA-p catalyst.
研究领域:
生物化学
·
催化化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ting Zhang,Wantong Zhao,Shiyan Li,Wenguang Cui,Baojun Wang,Yuefeng Liu,Riguang Zhang,Zhongkui Zhao
Selective transfer hydrogenation coupling of nitroarenes with benzyl alcohol is one of the most reliable strategies to access functionalized imines, but challenges remain, such as the multiple and complicated operate process, low reactivity, poor selectivity results from deep hydrogenation. Constructing highly efficient catalyst is critical for this organic transformation process. Herein, we propose a unique single-atom Co-N 4 sites on N-doped carbon, with significantly upshifted d -band center, fabricated by a one-pot solid-phase carbonization strategy, which generates an excellent catalyst for one-pot selective transfer hydrogenation coupling of nitroarenes with benzyl alcohol to various functionalized imines. Experimental and theoretical investigations demonstrate the clear linear correlation among the nitrobenzene turnover number ( TON ) and d -band center over the as-prepared Co based samples, indicating the vital effect of electronic structure of Co sites on catalytic performances. Furthermore, owing to the upshifted d -band center of Co-N 4 sites, thedesorption of aniline and N -benzylideneaniline is promoted, which accelerates the spontaneous condensation coupling of aniline with benzaldehyde and inhibits the deep hydrogenation of N -benzylideneaniline. Consequently, an outstanding catalytic performance with high activity and selectivity in transfer hydrogenation coupling for imine synthesis has been realized. This work not only presents a highly efficient non-precious metal catalyst for functionalized imines production, but also illustrates the critical effect of electron structure of metallic active site on catalytic properties and opens a new avenue for fabricating diverse single-atom catalysts for selective hydrogenation reactions.
研究领域:
化学
·
材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Yanan Sun,Xiangze Jia,Chin Ping Tan,Bin Zhang,Xiong Fu,Qiang Huang
The formation of inclusion complexes (ICs) between V-type starch and flavors is traditionally conducted in an aqueous system. In this study, limonene was solid encapsulated into V6-starch under ambient pressure (AP) and high hydrostatic pressure (HHP). The maximum loading capacity reached 639.0 mg/g after HHP treatment, and the highest encapsulation efficiency was 79.9 %. X-ray Diffraction (XRD) results showed that the ordered structure of V6-starch was ameliorated with limonene, which avoided the reduction of the space between adjacent helices within V6-starch generated by HHP treatment. Notably, HHP treatment may force molecular permeation of limonene from amorphous regions into inter-crystalline amorphous regions and crystalline regions as the Small-angle X-ray scattering (SAXS) patterns indicated, leading to better controlled-release behavior. Thermogravimetry analysis (TGA) revealed that the solid encapsulation of V-type starch improved the thermal stability of limonene. Further, the release kinetics study showed that a complex prepared with a mass ratio of 2:1 under HHP treatment sustainably released limonene over 96 h and exhibited a preferable antimicrobial effect, which could extend the shelf life of strawberries.
研究领域:
食品科学
·
生物学
✓ 已验证
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Zhe Dou,Pei-Ru Hu,Lin-Lin Song,Yi-Cheng Wang,Hao-Nan Tang,Zhen-Qi Weng,Ya-Jun Wang,Yuan-Qiang Cai
Carbonyl reductases (CRs) are promising biological macromolecules for the asymmetric synthesis of chiral secondary alcohols. A novel CR was evolved for efficient conversion of d -xylose into anti-aging ( S )-Pro-Xylane. Through extensive gene mining, an active carbonyl reductase Zm CR was identified from Zygofabospora marxiana with high reductive activity towards d -xylose-derived 1-C-(β- d -xylopyranosyl)-acetone (XPSA) and in situ cofactor regeneration capability. Using a three-round of concise engineering strategy, a hextuple mutant C85V/V128C/S129A/V161S/Y166H/T217A (M6) was identified from merely 157 mutants with specific activity of 46.00 U·mg −1 , about 306 folds of WT. The Shannon-Wiener index of M6 was 2.21, much higher than WT, indicating its extended substrate scope. M6 could efficiently catalyze the asymmetric reduction of 190 g·L −1 XPSA into ( S )-XPSP. The k cat / K M XPSA of M6 was 203.84 s −1 ·mM −1 , about 910 folds of WT. More non-bonded interactions were monitored in M6, contributing to the stabilization of reactive catalytic conformation. This study provides a promising biocatalyst for the chemoenzymatic synthesis of value-added anti-aging ( S )-Pro-Xylane from lignocellulosic d -xylose.
研究领域:
生物化学
·
酶工程
·
合成生物学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）