iScience
·
2023
·
IF 5.8
Fuhua Xu,Jiaying Yan,Yanlan Wang,Xiang Liu
Sodium formate (SF) is regarded as a technological additive to improve H 2 generation upon HCOOH dehydrogenation. The development of SF as a hydrogen storage material is still a challenge. Herein, we report the design and synthesis of carbon nanosphere-stabilized Pd nanoparticles (Pd/CNS) for the direct H 2 generation upon SF hydrolysis in the presence of Fe 3+ . The tandem reaction, isotopic mass spectrometry, and gas chromatograms result confirmed that SF hydrolysis generates H 2 with one H atom provided by SF and other H by H 2 O. The kinetic study and detailed mechanistic investigations have demonstrated that the concerted process between the cleavage of O-H bond in H 2 O and -O 2 C-H bond oxidative addition is the rate-controlling step in SF hydrolysis. This work offers a new chemical hydrogen storage material (HCOONa) for the high-efficiency generation, transport, and storage of H 2 .
研究领域:
化学
·
能源科学
·
催化科学
✓ 已验证
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Bin Hu,Wen-luan Xie,Yang Li,Zhen-xi Zhang,Ji Liu,Bing Zhang,Ti-peng Wang,Qiang Lu
The lignin pyrolysis process involves complex interaction reactions, where the bimolecular concerted interactions have been rarely studied. In the present work, an extended concerted interaction mechanism, hydroxyl-assisted hydrogen transfer (hydroxyl-AHT), was proposed based on the pyrolysis of the typical nonsubstituted and α-hydroxyl-substituted β-O-4 type lignin models (2-phenylethyl phenyl ether, PPE, and 2-phenoxy-1-phenylethanol, α-OH-PPE). This hydroxyl-AHT mechanism was investigated and confirmed with the combined fast pyrolysis experiments and quantum chemistry modeling. The results indicate that phenolic, watery, alcoholic, and enolic hydroxy compounds all can act as mediators for the concerted hydrogen transfer process in lignin pyrolysis and have similar assistant effects. Whereas, the hydroxyl-AHT has a great influence on the competitiveness of different concerted reactions to break the Cβ–O, Cα–Cβ, and Cα–OH bonds, respectively. To compare the pyrolysis of PPE and α-OH-PPE, the α-hydroxyl substituent leads to a significant promotion to the Cβ–O cleavage based on hydroxyl-AHT because there are more hydroxyl mediators and more concerted reaction types that can be involved in the bimolecular hydrogen transfer in α-OH-PPE pyrolysis. Hence, more phenol derived from the Cβ–O breakage was detected in the pyrolysis experiment of α-OH-PPE than that of PPE. In addition, this bimolecular hydroxyl-AHT interaction mechanism is universal in the concerted pyrolysis processes of lignin, also accelerating the cleavage of α-O-4 linkage, β-1 linkage, etc.
研究领域:
化学工程
·
能源科学
✓ 已验证
DOI
高影响因子
Water
·
2023
·Vol. 15
·期 9
·1758
·
IF 3.4
Hangli Zhang,Shujuan Wang,Ji Shu,Hongyu Wang
Doxycycline (DOX), a typical antibiotic, is harmful to aquatic ecosystems and human health. This study presents DOX removal by potassium ferrate (Fe(VI)) and montmorillonite and investigates the effect of Fe(VI) dosage, reaction time, initial pH value, montmorillonite dosage, adsorption pH, time and temperature on DOX removal. The results show that DOX removal increases when increasing the Fe(VI) dosage, with the optimal condition for DOX removal (~97%) by Fe(VI) observed under a molar ratio ([Fe(VI)]:[DOX]) of 30:1 at pH 7. The reaction of DOX with Fe(VI) obeyed second-order kinetics with a rate constant of 10.7 ± 0.45 M−1s−1at pH 7. The limited promotion (~4%) of DOX adsorption by montmorillonite was observed when the temperature increased and the pH decreased. Moreover, the synergetic effect of Fe(VI) and montmorillonite on DOX removal was obtained when comparing the various types of dosing sequences (Fe(VI) oxidation first and then adsorption; adsorption first and then Fe(VI) oxidation; simultaneous oxidation and adsorption). The best synergistic effect of DOX removal (97%) was observed under the simultaneous addition of Fe(VI) and montmorillonite, maintaining the Fe(VI) dosage (from 30:1 to 5:1). Five intermediates were detected during DOX degradation, and a plausible DOX degradation pathway was proposed.Keywords:advanced oxidation;potassium ferrate(VI);doxycycline degradation;synergistic reaction mechanism
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Li Ren,Jian Wang,Yaofeng Mao,Jie Chen,Yongjun Deng,Xingquan Zhang,Jun Wang
Aluminum (Al) is one of the most widely used metal fuels in the fields of automotive airbags, solid propellants, explosives and pyrotechnics. Unfortunately, it is hard to meet further demand of practical applications owing to the comparatively low calorific value. Herein, graphite fluoride (CF) and boron (B) are employed to construct Al/B/CF microspheres through self-assembly in emulsion to obtain high energy density and significantly improved combustion performance resulted from synergistic reaction between Al and B reacted with fluorine. The Al/B/CF microspheres with pore structure have uniformly distribution of components and the average size range from 60 to 600 μm. Based on the experimental results, CF content and Al/B mass ratio have significant important effects on the combustion behavior and pressure output. The highest burning rate (301.74 m/s) and pressurization rate (77.78 MPa/s) are obtained for the Al/B/CF microspheres with CF content of 50 wt% and Al/B mass ratio of 3 to 1, respectively. Furthermore, the combustion reaction process of single Al/B/CF microsphere are studied for the first time to understand the synergistic reaction between high reactivity of Al and high energy of B reacted with fluorine. This work demonstrates that introducing CF and B to construct Al/B/CF microspheres is an efficient strategy to achieve high energy density and reactivity for the practical applications.
研究领域:
材料科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED POWDER TECHNOLOGY
·
2025
·
IF 4.2
Jiaqi Wen,Chenghong Liu,Lihua Gao,Zhijun He
An oxidation roasting technology has been reported as an effective technology for successfully synthesizing nickel manganese ferrite Ni x Mn 1-x Fe 2 O 4 (0 < x < 1) with a spinel crystal structure. The experimental results demonstrated the successful synthesis of nickel manganese ferrite Ni 0.5 Mn 0.5 Fe 2 O 4 samples with relatively high purities at an oxidation roasting temperature of 1200 °C for 2 h with a Ni:Mn:Fe molar ratio of 1:1:4. The synthesized samples exhibited a magnetization saturation (Ms) value of 53.71 emu/g, a coercivity (Hc) value of 34.88 Oe, and a remanent magnetization (Mr) of 3.64 emu/g. Additionally, these samples had a total pore volume of 0.071 cm 3 /g, a Specific Surface Area (SSA) of 24.13 cm 2 /g, and an Average Particle Size (APS) of 12.32 nm. It was concluded that the synthesis route of Ni x Mn 1-x Fe 2 O 4 could be theoretically summarized into two routes. One route involves the simultaneous substitution of divalent iron (Fe 2+ ) and trivalent iron (Fe 3+ ) in the spinel structure of (Fe)[Fe] 2 O 4 by divalent manganese ions (Mn 2+ ) and trivalent nickel ions (Ni 3+ ), resulting in the formation of (Mn) x (Fe) 1-x [Ni] y [Fe] 2-y O 4 with a spinel crystal structure. In this structure, the Ni 3+ ions preferentially occupy the octahedral sites, whereas the Mn 2+ ions predominantly reside in the tetrahedral sites of the nickel manganese ferrites (Mn) x (Fe) 1-x [Ni] y [Fe] 2-y O 4 . Furthermore, the mixed spinel crystal structure of (Ni) y (Fe) 1-y [Mn] x [Fe] 2-x O 4 could be transformed into nickel manganese ferrite (Mn) x (Fe) 1-x [Ni] y [Fe] 2-y O 4 under the influence of a higher oxidization roasting temperature. Nickel manganese ferrite Ni x Mn 1-x Fe 2 O 4 (0 < x < 1) with normal and inverse spinel structures inevitably coexists and co-transformed in the synthesis process of Ni x Mn 1-x Fe 2 O 4 by oxidation roasting technology.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Ming Huang,Liang Zhu,Wenbiao Zhang,Lingjun Zhu,Zhongqing Ma,Dengyu Chen
Co-feeding of waste plastics during biomass catalytic fast pyrolysis can improve remarkably the yield of aromatic hydrocarbons. In this work, the simulated biomass by using its model components of cellulose, xylan, and lignin at different proportions was Co-CFP with LDPE to investigate the synergistic reaction mechanism between biomass and low-density polyethylene (LDPE) over hierarchical HZSM-5. Results showed that biomass and its model components were oxygen-enriched feedstock, while LDPE was the hydrogen-enriched feedstock with H/C eff over 2. The synergistic effect between biomass model components and LDPE was ordered as cellulose and LDPE > xylan and LDPE > lignin and LDPE. Because pyrolysis of cellulose produced higher yield of furans than that of xylan and lignin which acted as the key synergistic compounds in Diels-Alder reaction to form light aromatics. The transfer of hydrogen free radical from the LDPE-derived hydrocarbons to the biomass-derived oxygenates promoted the deoxygenation reaction of oxygenates in hierarchical HZSM-5. Diels-Alder reaction between furans and olefins was the key synergistic reaction which highly improved the yield of hydrocarbon aromatics. In general, the difference of the pyrolysis oxygenated intermediate among the biomass pseudo components resulted in different yields of light aromatics, where cellulose presented highest extent of synergistic reaction to LDPE.
研究领域:
能源化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yuqiang Ma,Zihang Zhao,Cong Zhang,Yijing Zhang,Chi Zhang,Jiachen Li,Ming Xu,Haixia Ma
Overall water splitting (OWS) involves two important half-reactions, namely hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). However, due to the high theoretical overpotential of OER, OWS needs to be realized with high energy consumption. Using anodic oxidation reaction with lower theoretical potential to replace oxygen evolution reaction (OER) can effectively reduce the energy consumption of overall water splitting (OWS) for hydrogen production. Here, we introduce a new oxidation reaction of green electrosynthesis of energetic materials (EMs) and coupled with OWS. The catalyst was prepared by electrodepositing Pt nanoparticles (Pt NPs) and Pt single atoms (Pt SAs) on MoS 2 nanosheets, which drives highly-efficient hydrogen production of 35.6 mV to drive 10 mA cm −2 . DFT calculations reveal the synergistic mechanism of Pt NPs and Pt SA/MoS 2 substrate for promoting hydrogen production, is that the energy barrier of water dissociation was reduced on the Pt NC sites and the produced H* migrated to the adjacent S sites for Heyrovsky step, while the Pt SA sites served as electron regulator for more thermoneutral H* adsorption on S sites, realizing the synergistic reaction kinetics in MoS 2 /Pt for promoting alkaline HER. Importantly, by integrating the OWS and electrosynthesis of 5,5′-azotetrazole (ZT) EMs, the cell voltage can be significantly reduced to 1.29 V at 10 mA cm −2 , realizing low-energy-consumption for hydrogen production. Meanwhile, the green electrosynthesis of ZT is achieved to avoid the hazardous process of traditional preparation methods. This study presents a new strategy for green electrosynthesis of EMs and low-energy-consumption hydrogen production.
研究领域:
能源化学
·
催化科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
COMBUSTION AND FLAME
·
2023
·
IF 4.4
Jian Wang,Jie Chen,Yaofeng Mao,Xingquan Zhang,Jun Wang,Fude Nie
Metal fuel with high energy and reactivity is an urgent need for the development of solid propellant, explosive and pyrotechnics. Herein, spherical B/Al/PTFE fuel is designed based on synergistic reaction effect between B/F and Al/F and prepared through the confinement-emulsion-templated method. The combustion reaction performance and pressure output performance of B/Al/PTFE microspheres are much better than their physically mixed counterparts. The synergistic reaction effect between B/F and Al/F on the reaction heat, flame propagation , and pressure output were systematically investigated through adjusting the B/Al mass ratio (30/0∼0/30). The DSC results show that the highest heat of combustion of 4904 J/g can be achieved when the B/Al mass ratio is 21/9. Furthermore, the combustion duration , peak pressure, and pressurization rate are monotonically accelerated from 653 ms, 352.15 kPa, and 305.67 MPa/s to 200 ms, 821.25 kPa, and 1831.18 MPa/s, respectively. This work provides a promising method for the design and preparation of highly composited metal fuel for practical application.
研究领域:
材料科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
CELLULOSE
·
2019
·Vol. 27
·期 3
·1799-1815
·
IF 3.917
Zhang Zheng,Dong Chaohong,Liu Jian,Kong Dezheng,Sun Ling,Lu Zhou
Abstract A novel compound containing silicon, phosphorus and nitrogen, named 1-(9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide)-4-(trimethoxysilylmethyl) piperazine (DOPO-PiP-Si), was synthesized as a reactive flame retardant and applied to prepare flame-retardant cotton fabrics. Its structure was characterized by Fourier transform infrared spectra, 1 H and 13 C nuclear magnetic resonance ( 1 H NMR and 13 C NMR), and flame retardancy of treated cotton fabrics was investigated thoroughly using the limited oxygen index (LOI), vertical burning test, thermogravimetric analysis and cone calorimetry test (CONE), respectively. The LOI value of the cotton fabrics treated with DOPO-PiP-Si increased to 27.6% and the char length decreased to 12.2 cm without afterflame and afterglow. From the results of CONE test, the peak heat release rate and total heat release of treated cotton fabrics decreased from 230.8 to 161.1 kW/m 2 and from 6.4 to 4.5 MJ/m 2 , respectively. Besides, the char residue reached 19.1%, which indicated that the treated cotton fabrics had excellent char formation ability and thermal stability. The morphology of char of the treated cotton fabrics was also characterized by scanning electron microscopy, it can be seen from results that the structure of fiber had no shrinkage and a few bubbles were distributed on the surface of fiber, which suggested that the treated cotton fabrics could display gas-phase flame retardant mechanism. Graphic abstract
研究领域:
材料科学
·
纺织工程
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 9
·1943-1955
·
IF 7.779
Yang Yang,Xiuzhen Zheng,Jiafang Liu,Zhulin Qi,Tianyue Su,Chun Cai,Xianliang Fu,Sugang Meng,Shifu Chen
To achieve high photocatalytic efficiency of H2 evolution, promoting the utilization rate of photogenerated charge carriers by photocatalytic synergistic reaction is an efficient strategy. In this work, Co3S4/Zn0.5Cd0.5S nanocomposites with Co3S4 derived from ZIF-67 were successfully prepared through a simple hydrothermal method. Under visible light irradiation, Co3S4/Zn0.5Cd0.5S exhibited high photocatalytic activities in a H2 production system coupled with selective oxidation of benzyl alcohol. Moreover, 3% Co3S4/Zn0.5Cd0.5S showed the optimal activity (7.67 mmol g−1 h−1), greatly improved compared to that of Zn0.5Cd0.5S (1.62 mmol g−1 h−1). The reasons for the improved photocatalytic performance were seriously investigated by a variety of measurements and can be attributed to the enhanced visible light absorption and more efficient electron–hole pair separation. This study provides a good strategy to construct photocatalysts with metal–organic frameworks (MOFs) and efficient charge separation for highly efficient H2 production.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2018
·Vol. 8
·期 17
·4463-4473
·
IF 5.365
Pengbo Hao,Mingjie Zhang,Wei Zhang,Zhiyang Tang,Ni Luo,Rong Tan,Donghong Yin
Keggin-type phosphotungstic acid (H3PW12O40, HPW)-based di-imidazolium ionic liquid (IL) hybrids were prepared by exchanging the protons of HPW with PEG-bridged di-imidazolium cations in water. Characterization results suggested that intact Keggin-type [PW12O40]3− anions were incorporated with various PEG-modified di-imidazolium cations through ionic interaction, giving PW-based ionic catalysts with a Gemini structure. PEG-bridged di-imidazolium cations could not only fine-tune the redox properties of PW anions but also enhanced the compatibility of the catalyst in the aqueous system, which in turn improved its catalytic performance. Furthermore, combination of double catalytic sites into a single molecule enforced an intramolecular, cooperative reaction pathway resulting in a further enhanced reaction rate and higher selectivity in the selective oxidation of benzyl alcohol with H2O2 in water. More importantly, the di-imidazolium IL cations imparted a reaction controlled phase transfer function to the PW hybrids. The catalysts were thus precipitated from the aqueous system upon consumption of H2O2 and could be reused several times without loss of activity and selectivity.
研究领域:
催化
·
化学工程
·
无机化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）