MONATSHEFTE FUR CHEMIE
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2018
·Vol. 149
·期 10
·1753-1758
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IF 1.285
Wei Ting,Zeng Yongming,Hong Liang,Zhang Hongxi,Wang Guozhen,Wang Shitao
Abstract A new phenanthroline derivative, [1,2,5]oxadiazolo[3′,4′:5,6]pyrazino[2,3- f ][1,10]phenanthroline was designed and synthesized. Its molecular structure was confirmed by single-crystal X-ray diffraction analysis. Its optoelectronic properties were systematically investigated by optical and electrochemical measurements. Thermogravimetric analysis revealed that the title compound is remarkably stable. Finally, DFT calculations further indicated that the phenanthroline derivative has potential applications in organic electronics. Graphical abstract
研究领域:
有机化学
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材料科学
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物理化学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Bin Han,Jianing Song,Shujie Liang,Weiyi Chen,Hong Deng,Xinwen Ou,Yi-Jun Xu,Zhang Lin
CO 2 adsorption is a critical step for CO 2 photoreduction, especially in diluted CO 2 , whereas an in-depth understanding of CO 2 adsorption effects is still lacking. Herein, isostructural NiCo 2 O 4 and MgCo 2 O 4 hierarchical hollow nanocages (NiCo 2 O 4 HCs and MgCo 2 O 4 HCs) have been ingeniously constructed for diluted CO 2 photoreduction. NiCo 2 O 4 HCs exerts an apparent quantum yield of 1.56% with CO selectivity of 89%, exceeding most previous inorganic catalysts in pure CO 2 . Nevertheless, MgCo 2 O 4 HCs is almost inert, even though it shows higher CO 2 uptake ability. DFT calculations results indicate that CO 2 molecule adsorbed on Ni sites can be readily reduced to CO, while the CO 2 on Mg sites cannot participate in this reaction. Therefore, only adsorbed CO 2 which can participate in reduction reactions, named active adsorption , can accelerate the whole reactions. This work unearths atomic-level insights into the relation between CO 2 adsorption and reduction, providing fundamental guidance to improve photocatalytic performance.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Xiaoyue Chen,Songge Zhang,Xiu Qian,Zhangqian Liang,Yanjun Xue,Xiaoli Zhang,Jian Tian,Ye Han,Minhua Shao
Herein, we assemble semi-metallic 1T′ phase MoS 2 on the surface Ti 3 C 2 MXene (1T′-MoS 2 /Ti 3 C 2 composite) by one-step hydrothermal method for nitrogen fixation. 1T′-MoS 2 /Ti 3 C 2 composites present a high ammonia yield rate of 31.96 µg h −1 mg −1 cat. at − 0.95 V vs. RHE and a Faradaic efficiency (FE) of 30.75% at − 0.7 V, which is much better than pure 1T′-MoS 2 and pure Ti 3 C 2 MXenes alone. Furthermore, the 1T′-MoS 2 /Ti 3 C 2 composites exhibit good selectivity and stability with no significant decrease in ammonia yield rate and FE. Density functional theory (DFT) calculations reveal that 1T′-MoS 2 /Ti 3 C 2 composite makes the activation and further reduction of *N 2 more thermodynamically favorable than pure 1T′-MoS 2 . 1 5 N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N 2 in the electrolyte.
研究领域:
材料科学
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电催化
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理论计算
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DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2018
·Vol. 24
·期 19
·4902-4908
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IF 5.16
Yu-Ping Qiu,Hui Yin,Hao Dai,Li-Yong Gan,Hong-Bin Dai,Ping Wang
Graphical Are two metals better than one? Surface modification of a Ni nanocatalyst by Ir results in remarkably improved catalytic properties towards H 2 generation from N 2 H 4 ⋅ H 2 O. Coupled experimental and theoretical studies reveal that the formation of Ni−Ir alloy on the catalyst surface plays a crucial role in determining the catalytic performance (see figure). Selective decomposition of hydrous hydrazine (N 2 H 4 ⋅ H 2 O) over metal catalysts provides a promising means for onboard or portable hydrogen source applications. Studies on N 2 H 4 ⋅ H 2 O decomposition catalysts mainly focus on the effects of bulk composition and structure on their performances, instead of the surface-composition-dependent properties. Herein, the synthesis of an Ir-modified Ni/ meso -CeO 2 catalyst is reported by using a combination of colloidal solution combustion synthesis and galvanic replacement methods. A combination of structural characterization, control experiments, and DFT calculations reveals that the Ni−Ir alloy resulting from calcination treatment exerts a profound effect on the catalytic properties. The resulting Ni@Ni−Ir/ meso -CeO 2 catalyst shows excellent catalytic performance towards hydrogen generation from N 2 H 4 ⋅ H 2 O, which compares favorably with the Ni−Ir bimetallic catalysts reported to date.
研究领域:
材料科学
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催化化学
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理论计算化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Yan Wu,Tao Liu,Bin Ji,Wei Wang
Iron-cobalt alloy is a potential and economical magnetostrictive material, however, our microscopic understanding of the co-electrodeposition process of Fe-Co alloys is still unsatisfactory. In this work, a flat Fe-Co film with 10 μm was successfully prepared by electrodeposition with a non-toxic sulfate solution. The effects of (NH 4 ) 2 SO 4 , an important additive, were studied and DFT calculation was used to analyze the mechanism of (NH 4 ) 2 SO 4 . EIS shows that (NH 4 ) 2 SO 4 can promote the Fe-Co co-deposition process and obviously inhibits the hydrogen evolution reaction. In addition, (NH 4 ) 2 SO 4 can significantly reduce the internal stress of the Fe-Co film by 110,000 MPa, so that the cracks caused by the internal stress are obviously removed. The results of quantum chemistry calculation further show that NH 4 + is more inclined to adsorb on Fe-Co surface than H 2 O and H + , which reduces the hydrogen evolution on the electrode surface. The results are beneficial to improve the Fe-Co co-deposition process, reduce the internal stress and to prepare a high-performance Fe-Co magnetic film. The films will be assembled on the electronic devices with sensors.
研究领域:
材料科学
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电化学
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表面化学
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量子化学
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DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2023
·
IF 8.7
Chen Yang,Jian Yang,Shuangshuang Liu,Mingxue Zhao,Xu Duan,Hongli Wu,Lang Liu,Weizao Liu,Jiangling Li,Shan Ren,Qingcai Liu
Owing to its feasibility, efficiency in light-harvesting and effectiveness in the interfacial charge transfer between two n-type semiconductors, constructing heterojunction photocatalysts have been identified as an effective way for enhancing the photocatalytic properties. In this research, a C–O bridged CeO 2 /g-C 3 N 4 (cCN) Step-scheme (S-scheme) heterojunction photocatalyst was constructed successfully. Under visible light irradiation, the cCN heterojunction exhibited the photocatalytic degradation efficiency of methyl orange, which was about 4.5 and 1.5 times higher than that of pristine CeO 2 and CN, respectively. The DFT calculations, XPS and FTIR analyses demonstrated the formation of C–O linkages. And the calculations of work functions revealed the electrons would flow from g-C 3 N 4 to CeO 2 due to the difference in Fermi levels , resulting in the production of internal electric fields . Benefiting from the C–O bond and internal electric field, the photo-induced holes in the valence band of g-C 3 N 4 and the photo-induced electrons from conduction band of CeO 2 would be recombined when exposed to visible light irradiation, while leaving the electrons with higher redox potential in the conduction band of g-C 3 N 4 . This collaboration accelerated the separation and transfer rate of photo-generated electron-hole pairs, which promoted the generation of superoxide radical (•O 2 − ) and improved the photocatalytic activity .
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Journal of CO2 Utilization
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2022
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IF 8.321
Shujie Liang,Gongchang Zeng,Xiaohui Zhong,Hong Deng,Zuqi Zhong,Zhang Lin,Jianlin Huang
Photoreduction of diluted CO 2 is an effective strategy for the sustainable and environmentally friendly development of energy. In this study, lattice strain in NiSe is modulated through the control of the Ni concentration for the photoreduction of diluted CO 2 . Refined XRD data and the results of the Williamson–Hall analysis indicate that the lattice strain is induced by lattice distortion caused by an absence of Ni atoms in the crystal lattice . In pure CO 2 , the cumulative CO yield and selectivity of Ni 1−x Se nanoflowers reached approximately 19.39 µmol and 90.7 % in 3 h, respectively. For lower CO 2 concentrations of 0.1 and 0.05 atm, the CO selectivity of Ni 1−x Se was approximately 72.7 % and 61.7 %, respectively. On characterization of the synthesized nanoflowers , we deduced that the lattice-strained Ni 1−x Se exhibited a favorable electronic band structure that improved the separation efficiency of the photogenerated carriers . DFT calculations results revealed that the lattice strain significantly facilitated the adsorption and activation of CO 2 , which resulted in highly efficient CO 2 photoreduction. This study provides an effective strategy for the design and synthesis of high-performance catalysts based on the modification of their crystal structures.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
RSC Advances
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2023
·Vol. 13
·期 13
·8915-8922
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IF 3.9
Tong Zhou,Haitang Wei,Bin Xiao,Tianping Lv,Liangfei Duan,Qingjie Lu,Jin Zhang,Yumin Zhang,Qingju Liu
One of the most promising strategies for producing hydrogen is photocatalytic water splitting, in which the photocatalyst is a key component. Among many semiconductor photocatalysts, g-C3N4 has attracted great attention due to its narrow band gap, excellent stability and low cost. However, practical application is limited by its poor intrinsic activity. In this work, a high-performance porous g-C3N4 (PCN) photocatalyst with anchored Cu single atoms (CuSAs) was synthesized by a one-step co-heating approach. The obtained Cu1.5–PCN displays an excellent hydrogen evolution rate (HER) of 2142.4 μmol h−1 g−1 under visible light (=420 nm), which is around 15 and 109 times higher than those of PCN and bulk g-C3N4, respectively. In addition, it also shows good stability during H2 evolution. The results of experimental research and DFT simulations indicate that the single Cu ions formed bonds with the N-ring and these remain stable. Meanwhile, the special electronic structure of the Cu–N charge bridge extends the light absorption band to the visible-light region (380–700 nm). This high-performance and low-cost photocatalyst has great potential in solar energy conversion.
研究领域:
材料科学
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能源化学
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DOI
PubMed
高影响因子
Small
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2023
·Vol. 20
·期 3
·2304990
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IF 13.3
Na Ye,Wenchao Sheng,Riguang Zhang,Binhang Yan,Zhao Jiang,Tao Fang
The splitting of the C–C bonds of ethanol remains a key issue to be addressed, despite tremendous efforts made over the past several decades. This study highlights the enhancement mechanism of inexpensive NbN-modified Pd 1 Sn 3 -NbN/C towards the C–C bonds cleavage for alkaline ethanol oxidation reaction (EOR). The optimal Pd 1 Sn 3 -NbN/C delivers a catalytic activity up to 43.5 times higher than that of commercial Pd/C and high carbonate selectivity (20.5%) toward alkaline EOR. Most impressively, the Pd 1 Sn 3 -NbN/C presents good durability even after 25 200 s of chronoamperometric testing. The enhanced catalytic performance is mainly due to the interfacial interaction between PdSn and NbN, demonstrated by multiple structural characterization results. In addition, in situ ATR-SEIRAS (Attenuated total reflection-surface enhanced infrared absorption spectroscopy) results suggest that NbN facilitates the C–C bonds cleavage towards the alkaline EOR, followed by the enhanced OH adsorption to promote the subsequent oxidation of C1 intermediates after doping Sn. DFT (density functional theory) calculations indicate that the activation barriers of the C–H bond cleavage in CH 3 CH 2 OH, CH 3 CHOH, CH 3 CHO, CH 3 CO, CH 2 CO, and the C–C bond cleavage in CH 3 CO, CH 2 CO, CHCO are evidently reduced and the removal of adsorbed CH 3 CO and CO becomes easier on the PdSn-NbN/C catalyst surface.
研究领域:
材料科学
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电化学
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表面科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Qi-Su Huang,Wei Wu,Wei Wei,Lan Song,Jing Sun,Bing-Jie Ni
As one of the most toxic heavy metals, lead ions (Pb 2+ ) contamination arouses increasing public concern for high carcinogenicity and neurotoxicity. In this study, a modified hydrothermal method was designed to fabricate novel hexagonal K 2 W 4 O 13 nanowires to achieve highly-efficient Pb 2+ removal from water. Attractively, the as-prepared K 2 W 4 O 13 exhibited large uptake capacity (228.83 mg/g), fast kinetic (141.67 mg/g in 30 min), superior acid-resistance (75% of removal at pH = 2) and excellent reusability (over 95% of removal after 5 runs) toward Pb 2+ adsorption. The Langmuir isotherm and pseudo-second-order kinetic model gave a better fit to the adsorption experimental data. The Pb 2+ adsorption process on K 2 W 4 O 13 was revealed to be a spontaneous, exothermic, film diffusion limited chemisorption reaction. The mechanism studied elucidated that both ion-exchange and complexation were involved in Pb 2+ adsorption, with each accounting for approximate 50% of Pb 2+ elimination. Through density functional theory (DFT) calculation, the equatorial oxygen was found to be more accessible for Pb attachment than the axial corner oxygen from [WO 6 ] octahedra. Electron pairs from the adjacent O atoms would transfer to the empty orbitals of Pb atoms after adsorption, causing the Pb 2+ removal via metal-ligand complexation.
研究领域:
环境科学
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材料科学
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化学
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DOI
高影响因子
Nanomaterials
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2026
·Vol. 16
·期 2
·128
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IF 4.3
Bo Li,Nanhui Zhang,Yuxing Lei,Mengmeng Zhu,Haitao Yang
Electric-field-sensitive dielectrics play a crucial role in electric field induction sensing and related capacitive conversion, with interfacial polarization and charge accumulation largely determining the signal output. This paper introduces graphene/transition metal dichalcogenide (TMD) (MoSe 2 , MoS 2 , and WS 2 ) heterojunctions as functional fillers to enhance the dielectric response and electric-field-induced voltage output of flexible polydimethylsiloxane (PDMS) composites. Density functional theory (DFT) calculations were used to evaluate the stability of the heterojunctions and interfacial electronic modulation, including binding behavior, charge redistribution, and Fermi level-referenced band structure/total density of states (TDOS) characteristics. The calculations show that the graphene/TMD interface is primarily controlled by van der Waals forces, exhibiting negative binding energy and significant interfacial charge rearrangement. Based on these theoretical results, graphene/TMD heterojunction powders were synthesized and incorporated into polydimethylsiloxane (PDMS). Structural characterization confirmed the presence of face-to-face interfacial contacts and consistent elemental co-localization within the heterojunction filler. Dielectric spectroscopy analysis revealed an overall improvement in the dielectric constant of the composite materials while maintaining a stable loss trend within the studied frequency range. More importantly, calibrated electric field induction tests (based on pure PDMS) showed a significant enhancement in the voltage response of all heterojunction composite materials, with the WS 2 -G/PDMS system exhibiting the best performance, exhibiting an electric-field-induced voltage amplitude 7.607% higher than that of pure PDMS. This work establishes a microscopic-to-macroscopic correlation between interfacial electronic modulation and electric-field-sensitive dielectric properties, providing a feasible interface engineering strategy for high-performance flexible dielectric sensing materials.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Wenfeng Han,Bing Liu,Yikun Kang,Zhikun Wang,Wei Yu,Hong Yang,Yongnan Liu,Jiaqin Lu,Haodong Tang,Ying Li,Weiyu Song
Vinylidene fluoride (VDF) is one of the major fluorinated monomers. Currently, it is produced via the pyrolysis of 1-chloro-1,1-difluoroethane at above 650 °C without any catalyst. Herein, we propose that metal fluorides are promising catalysts that selectively promote the pyrolysis at 300–450 °C. With various metal fluorides as the catalysts, the conversion rate increases with the amount of acidic sites, which is also reinforced by the Bader charges q. The affinity to Cl of the metal fluorides is responsible for the selectivity. However, the high affinity to Cl also leads to the chlorination of metal fluorides forming metal chlorides followed by the deactivation of the catalyst. Different from other metal fluorides, F defects play a major role in the performance of AlF3. With an increase in F defects, the selectivity changes from vinylidene chlorofluoride (dehydrofluorination) to VDF (dehydrochlorination), which further confirms the role of affinity to Cl in the selectivity.
研究领域:
物理化学
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催化化学
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材料化学
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有机氟化学
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反应机理研究
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）