CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yachao Xu,Zhong Zhou,Peng Yu,Ying Wang
Synergistically tuning electronic states at the atomic level to facilitate photocatalytic overall water splitting is a challenge. However, elucidation of the role of specific electronic states of Znln 2 S 4 (ZIS) in regulating both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) is still scarce, making it difficult to accurately predict the actual photocatalytic performance. Here, the substitution of Zn sites with Al atoms was found to modulate the potential difference of the ZIS surface domain heterojunction structure, and electrons were further transferred to CuS to form a built-in field that promotes charge separation. When Al doping is present on the ZIS surface, ZIS exhibits p-type semiconductor properties, which leads to the formation of p-n junctions within Al-CuS/ZIS itself. Due to the large work function and metallic properties of CuS, and Al-CuS/ZIS as a whole tends to form a Schottky heterojunction, and the two heterojunction structures synergistically promote the migration of photogenerated carriers. In addition, the Al doping changes the electronic states around the ZIS, allowing the Al ZIS to promote the adsorption of O* and H* during OWS. The solar-driven photocatalytic overall water splitting efficiency of Al-CuS/ZIS is as high as 153.6 (HER) and 73.1 (OER) μmol/h g −1 , which is about 10 times that of ZIS. This work opens the possibility to design efficient photocatalytic materials through tunable composition and electronic structure.
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Nanomaterials
·
2023
·Vol. 13
·期 12
·1837
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IF 5.3
Miaomiao Jin,Zhanxin Song,Wei Liu,Guozhen Wang,Mo Xian
Biological approaches for the synthesis of a hybrid explosive–nanothermite energetic composite have attracted greater scientific attention because of their advantages, including their moderate reactions and the absence of secondary pollution. In this study, a simple technique was developed to fabricate a hybrid explosive–nanothermite energetic composite based on a peptide and a mussel-inspired surface modification. Polydopamine (PDA) was easily imprinted onto the HMX, where it maintained its reactivity and was capable of reacting with a specific peptide used to introduce Al and CuO NPs to the surface of the HMX via specific recognition. The hybrid explosive–nanothermite energetic composites were characterized using differential scanning calorimetry (TG-DSC), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy(XPS), and a fluorescence microscope. A thermal analysis was utilized to investigate the energy-release properties of the materials. The[email protected]@CuO, which benefitted from an enhanced interfacial contact in comparison with the physically mixed sample (HMX-Al-CuO), demonstrated a 41% lower HMX activation energy.Keywords:biological self-assembly;polydopamine;peptide;green preparation;activation energy
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Yong Zhang,Siqi Huang,Bingyu Mei,Lingyi Jia,Jun Liao,Wenkun Zhu
A novel dopamine-supported Mg( Ca )Al layered double hydroxide composite was synthesized by co-precipitation method. The existence of Ca 2+ and dopamine could promote the capture of uranium on the layered double hydroxides. In batch experiments, the composite exhibited good uranium removal performance, including high adsorption capacity (687.3 mg/g), strong anti-interference and good reusability (the removal percentage was still higher than 90 % after five cycles). At low initial uranium concentration, the uranium removal percentage on the composite exceeded 99.7 % and the residual concentration of uranium in the solution was <0.03 mg/L, reaching the limited standard of the World Health Organization. The studies of adsorption kinetics and isotherm indicated that the uranium adsorption behavior on the composite conformed to the pseudo-second-order kinetic and Langmuir isotherm models, suggesting that the process was a monolayer adsorption dominated by chemical adsorption. Furthermore, the high-efficiency uranium adsorption on the Mg( Ca )Al layered double hydroxide was mainly attributed to the strong complexation between the active sites (-OH and -NH 2 ) and uranium, the precipitation of interlayer intercalation ions (CO 3 2− and OH − ) to uranium and the ion exchange of Ca 2+ to uranium. Due to these advantages, the dopamine-supported Mg( Ca )Al layered double hydroxide composite is expected to be used as fine adsorbent to remove uranium from wastewater.
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MATERIALS CHARACTERIZATION
·
2023
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IF 4.7
Chengyi Xu,Xiaoping Cai,Xinyang Jiao,Khanh Ly Vu,Zhichao Shang,Peizhong Feng
Porous CoAl 3 intermetallics have great catalytic potential. However, its high porosity and controllable preparation are still incipient. In this paper, the effect of isothermal treatment on the near-net formation process of porous CoAl 3 material is studied, and the phase transformation process and diffusion kinetics of the Co/Al diffusion couple in the solid-phase diffusion stage are described. The results show that isothermal treatments in the range of 510–550 °C reduce the exothermic intensity of the thermal explosion (TE) reaction. The holding time of 30 min at 530 °C facilitates the near-net formation of porous CoAl 3 . The isothermal treatment does not affect the phase composition of the final product. Still, it causes changes in the phase and depth of the diffusion, affecting the exothermic strength and skeleton morphology. Based on the phase transition and thermodynamic analysis , the CoAl phase formation is the key to reducing the exothermic intensity. The diffusion kinetics indicates that the low diffusion activation energy of the CoAl phase (Q 1 = 1.66 kJ mol −1 ) is the main reason for the preferential formation. And the exponential kinetic factor of the second diffusion layer (n 2 = 0.75) explains its high diffusion depth.
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CARBOHYDRATE POLYMERS
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2018
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IF 5.158
Wenbin Hu,Lingbin Lu,Zhanying Li,Lin Shao
Bulk Al-doped carboxymethyl cellulose aerogels were obtained via a facile slow-gel method and freeze-drying technology. In this method, the cross-linker Al 3+ was released slowly and completely with enough d -(+)-gluconic acid δ -lactone as a sustained-release agent. Depended on controlled releasing of Al 3+ , the reaction speed between Al 3+ and carboxyl groups was controlled and Al 3+ was well-distributed in the aerogels. The coordination type between Al 3+ and carboxymethyl cellulose was the bidentate bridging coordination. By adjusting the amount of Al 3+ and the degree of substitution of carboxymethyl cellulose, interconnected network and closely packed sheet-like structure presented, respectively. According to the nitrogen adsorption-desorption isotherms, the aerogels were a kind of mesoporous material with pore blocking or cavitation. In addition, the aerogels exhibited outstanding weight-bearing capacity and excellent flame retardancy. This work provided a valuable reference for doping metal ions into polysaccharide aerogels and expanding the application fields of aerogels.
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CERAMICS INTERNATIONAL
·
2019
·
IF 3.45
Hang Liu,Shengqiang Song,Andrie M. Garbers-Craig,Zhengliang Xue
Cr 2 O 3 is a well-known corrosion resistant oxide used in refractory applications. However, it can oxidize into toxic and water-soluble Cr(VI) compounds upon reaction with calcium aluminate cement phases in the presence of oxygen, which subsequently causes disposal problems after use. This study describes the extent to which chromium in the spinel Mg(Al,Cr) 2 O 4 phase can be oxidized to Cr(VI) when it reacts with the calcium aluminate cement phases C 12 A 7 , CA, CA 2 and free CaO at 1300 °C in air, using XRD, XPS and leaching tests (TRGS 613 standard) as analytical tools. On reaction with CaO, the Mg(Al,Cr III ) 2 O 4 spinel mainly transformed into hauyne (Ca 4 Al 6 Cr VI O 16 ) and Ca 5 Cr 3 O 12 which contains both Cr(IV) and Cr(VI). The reaction of C 12 A 7 and CA with the spinel phase also resulted in the formation of Ca 4 Al 6 CrO 16 . Conversely, the reaction of Mg(Al,Cr III ) 2 O 4 spinel with CA 2 resulted in the formation of only a trace amount of Cr(VI). Water-soluble Cr(VI) leached in large quantities (>100 mg/L) from samples where the Mg(Al,Cr III ) 2 O 4 reacted with either C 12 A 7 or CA. Almost no Cr(VI) leached from the sample when Mg(Al,Cr III ) 2 O 4 reacted with CaO, using the standard TRGS 613 leach test, but a significant amount of Cr(VI) was released into solution when leached with a HCl solution for 12 h. Both Cr(IV) and Cr(VI) present in the Ca 5 Cr 3 O 12 dissolved into acidic solution. Only a small amount of Cr(VI) leached from the sample that resulted when spinel was reacted with CA 2 , even after a prolonged HCl leach. Cr(III) in spinel Mg(Al,Cr) 2 O 4 is very stable and does not leach in either distilled water or acidic solution.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2019
·Vol. 166
·期 2
·D65
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IF 3.12
Min Li,Ying Li,Zhaowen Wang
The electrochemical reduction of zirconium oxide in a molten salt of 2.4NaF·AlF3 (molar ratio = 2.4) was studied at 1273 K. Cyclic voltammetry results show that Zr(IV) ions are first reduced to an intermediate valence and, then, are co-deposited with aluminum to form an Al-Zr alloy. Potentiostatic electrolysis experiments were carried out at different potentials (−0.95 and −1.25 V) and at 1273 K, and the electrolysis products were characterized using SEM-EDS and XRD. The XRD analysis confirms that a mixture of cryolite molten salt and ZrO2 was electrodeposited at −0.95 V, while aluminum and Al3Zr were electrodeposited at −1.25 V. The SEM analysis shows that the aluminum and Al3Zr were in two different phases.
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POLYHEDRON
·
2019
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IF 2.284
Ning Tian,Yifang Dai,Qing Liu,Wei Dai
A general synthetic strategy for HS-Fe 3 O 4 @MIL-53(Al) adsorbent has been developed in this work. The composite material exhibits an efficient capture performance for rubidium ion due to sulfhydryl group and magnetic Fe 3 O 4 doped in its porous cavity. The results of X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy, and N 2 adsorption–desorption proved that the HS-Fe 3 O 4 was immobilized in the composite material. High Rb + uptake capacity over the HS-Fe 3 O 4 @MIL-53(Al) is attributed to the exchange of acidic protons between the sulfhydryl group and the Rb + . The pseudo-second-order and Freundlich model could make a good description of the adsorption process. The Rb + sorption selectivity was moderately influenced by any co-ions effect (K + , Na + and Cs + ) due to HS-Fe 3 O 4 doped. These results reveal that our novel composite material might be a promising industrial adsorbent for Rb + capture.
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JOURNAL OF APPLIED PHYSICS
·
2018
·Vol. 123
·期 9
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IF 2.176
Ma Xiaoxia,Cheng Shengxian,Hu Yan,Ye Yinghua,Shen Ruiqi
The integration of composite energetic films (CEFs) with various types of initiators can effectively adjust their performance and represents potential applications in microscale energy-demanding systems. In this study, the Al/Bi 2 O 3 /graphene oxide (GO) CEFs were successfully integrated into copper micro-ignitors by electrophoretic deposition, a low-cost and time-saving method. The effects of the Al/Bi 2 O 3 /GO CEFs with different GO contents on exothermic performance and ignition properties of micro-ignitors were then systematically investigated in terms of heat release, activation energy, ignition duration, the maximum height of the ignition product, and ignition delay time. The results showed that the addition of GO promoted more heat releases and higher activation energies of Al/Bi 2 O 3 /GO CEFs. The addition of ≤3.5 wt. % GO prolonged the ignition duration from 450 μ s to 950 μ s and increased the maximum height of the ignition product from about 40 mm to 60 mm. However, the micro-ignitors with more than 3.5 wt. % GO cannot be ignited, which suggested that GO played a contradictory role in the ignition properties of micro-ignitors and the controlled GO content was a prerequisite for improved ignition performance. The ignition delay time gradually extended from 10.7 μ s to 27.6 μ s with increases in the GO contents of Al/Bi 2 O 3 CEFs, revealing that an increase in the weight ratio of GO leads to lower ignition sensitivity of micro-ignitors.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Yanhui Cao,Dajiang Zheng,Xueliang Li,Jinyan Lin,Cheng Wang,Shigang Dong,Changjian Lin
A superhydrophobic ZnAl–layered double hydroxide (LDH)–La film was prepared by a hydrothermal method and further modification by laurate anions in this work. Comprehensive characterizations of this film were performed in terms of morphology, composition, structure, roughness, and wettability by scanning electronic microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, three-dimensional laser scanning confocal microscopy. The long-term corrosion protection effect of this superhydrophobic film was investigated deeply by monitoring the changes of the electrochemical impedance spectra for a long time of up to a month in 3.5 wt % NaCl solution. In the meantime, the changes of the contact angle were also recorded with the evolution of the immersion time. The result indicated that the stable superhydrophobic ZnAl–LDH–La film was able to provide efficient protection for the underlying Al substrate for a long time. In addition, the capability of the superhydrophobic surface against harsh conditions, including chemical damages and physical damages, was emphatically investigated. It was found that the superhydrophobic surface was chemically stable toward acid (pH ≥ 3), alkali, and heating, and it also exhibited high ultraviolet (UV) radiation resistance. This superhydrophobic coating maintained superhydrophobicity for 7 days of radiation in an UV chamber equipped with a 40 W UV lamp (λ = 254 nm), indicating superior ability of adapting to outdoor environment. This comprehensive investigation of the superhydrophobic ZnAl–LDH–La film is considerably helpful for researchers and engineers to get deep insight into its potential for practical applications in the field of corrosion and protection.
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DALTON TRANSACTIONS
·
2018
·Vol. 48
·期 2
·426-434
·
IF 4.099
Yiyue Zhang,Liangjing Zhang,Liang Hu,Shaolong Huang,Zhengyuan Jin,Min Zhang,Xiaoyong Huang,Jianguo Lu,Shuangchen Ruan,Yu-Jia Zeng
Surface-enhanced Raman scattering (SERS) and surface-enhanced infrared absorption (SEIRA) are complementary techniques, and both provide fingerprint structural information on various materials with a high sensitivity. Herein, Zn–Al layered double hydroxides (LDHs) are proposed for the first time as highly sensitive and uniform substrates for both SERS and SEIRA. Zn–Al LDHs show a remarkable SERS effect with an enhancement factor (EF) as high as 1.637 × 104 by using 4-mercaptobenzoic acid (4-MBA) as the probe molecule, where the charge transfer and hydrogen bonds are believed to result in the SERS effect. Interestingly, Zn–Al LDHs also exhibit SEIRA by using 4-methoxybenzenethiol (4-MTP), where the resultant substrates possess excellent long-term stability. This study not only presents a facile route to fabricate LDH materials, but also provides a novel substrate that can be used in both SERS and SEIRA.
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ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Fufeng Cai,Xianghai Song,Yuanfeng Wu,Jun Zhang,Guomin Xiao
In this study, different acid-modified Co–Al catalysts were prepared and employed for glycerol hydrogenolysis by the addition of B, Ce, Zr, and heteropolyacids (HSiW, HPW, HPMo) to Co–Al catalysts. The catalysts prepared in this work were thoroughly examined by various characterization methods such as BET, ICP, SEM, H2 chemisorption, TEM, XRD, H2-TPR, NH3-TPD, XPS, and FTIR. The results showed an increase in the acid strength and Co dispersion on the catalytic surface for the modified Co–Al catalysts. This facilitated the conversion of glycerol. When ethanol was used as a solvent, the selectivity of 1,2-propanediol (1,2-PDO) by the acid-modified Co–Al catalysts decreased slightly, attributable to the enhanced etherification activity of glycerol with ethanol. However, when water was used as a solvent, the modified Co–Al catalyst with the B, Ce, and Zr species increased the selectivity of 1,2-PDO. Addition of heteropolyacids to the Co–Al catalyst enhanced the selectivity of 1,3-propanediol (1,3-PDO) as compared to 1,2-PDO selectivity which was relatively low due to its association with Brønsted acid sites on the modified Co–Al catalysts. The optimal HSiW/Co–Al catalyst (in terms of both 1,2- and 1,3-PDO selectivity) showed 76.3% glycerol conversion and 18.3% 1,3-PDO selectivity with a good stability. This could be attributed to the existence of well-dispersed Co particles with strong interaction between Co and W species.
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