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Removal of ammonium and nitrate through Anammox and FeS-driven autotrophic denitrification

《环境科学与工程前沿（英文）》 2023年第17卷第6期 doi: 10.1007/s11783-023-1674-4

摘要：

● Simultaneous NH₄⁺/NO₃^– removal was achieved in the FeS denitrification system

关键词： Anammox Denitrification FeS NH₄⁺/NO₃⁻ Sulfammox

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以NH3sub>OH+sup>/NH2sub>NH3sub>+sup>作为B位阳离子的无金属六方钙钛矿含能材料 Article

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

《工程（英文）》 2020年第6卷第9期页码 1013-1018 doi: 10.1016/j.eng.2020.05.018

摘要：文中通过合理地选择分子组分，经由易于规模放大的简单合成路线，以NH3sub>OH+sup>和NH2sub>NH3sub>+sup>分别作为B位点阳离子构筑了两例无金属六方钙钛矿含能材料(H2sub>dabco)B(ClO4sub>)3sub>（分别命名为DAP-6和DAP-7，其中H2sub>dabco2+sup>是1,4-二氮杂双环[2.2.2]辛烷-1,4-二鎓离子）。与基于NH4sub>+sup>阳离子构筑的立方钙钛矿类似物(H2sub>dabco)(NH4sub>)(ClO4sub>)3sub>相比，DAP-6和DAP-7有较高的晶体堆积密度和生成焓，从而具有更高的爆轰性能。

关键词：含能材料单质炸药固体推进剂无金属六方钙钛矿

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On the monolayer dispersion behavior of Co3sub>O4sub> on HZSM-5 support: designing applicable

《化学科学与工程前沿（英文）》 2023年第17卷第11期页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要： Based on monolayer dispersion theory, Co₃O₄/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co₃O₄ can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m^–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O₂^–) and acid sites are crucial for the reaction, which can adsorb and activate NO_x and NH₃ reactants effectively. Below the monolayer dispersion threshold, Co₃O₄ is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co₃O₄ above the capacity is harmful to the reaction performance. 4% Co₃O₄/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O₂^– species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co₃O₄/ZSM-5 catalyst can be prepared by loading the capacity amount of Co₃O₄ onto HZSM-5 support.

关键词： Co₃O₄/ZSM-5 NO_x-SCR by NH₃ monolayer dispersion threshold effect surface acid sites surface active O₂^– anions

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Enabling nickel ferrocyanide nanoparticles for high-performance ammonium ion storage

《化学科学与工程前沿（英文）》 2023年第17卷第2期页码 226-235 doi: 10.1007/s11705-022-2198-3

摘要： Prussian blue and its analogs are extensively investigated as a cathode for ammonium-ion batteries. However, they often suffer from poor electronic conductivity. Here, we report a Ni₂Fe(CN)₆/multiwalled carbon nanotube composite electrode material, which is prepared using a simple coprecipitation approach. The obtained material consists of nanoparticles with sizes 30–50 nm and the multiwalled carbon nanotube embedded in it. The existence of multiwalled carbon nanotube ensures that the Ni₂Fe(CN)₆/multiwalled carbon nanotube composite shows excellent electrochemical performance, achieving a discharge capacity of 55.1 mAh·g^–1 at 1 C and 43.2 mAh·g^–1 even at 15 C. An increase in the ammonium-ion diffusion coefficient and ionic/electron conductivity based on kinetic investigations accounts for their high performance. Furthermore, detailed ex situ characterizations demonstrate that Ni₂Fe(CN)₆/multiwalled carbon nanotube composite offers three advantages: negligible lattice expansion during cycling, stable structure, and the reversible redox couple. Therefore, the Ni₂Fe(CN)₆/multiwalled carbon nanotube composite presents a long cycling life and high rate capacity. Finally, our study reports a desirable material for ammonium-ion batteries and provides a practical approach for improving the electrochemical performance of Prussian blue and its analogs.

关键词： nickel ferrocyanides NH₄⁺ electrochemistry Prussian blue aqueous ammonium ion batteries

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从氢原子质子化模型计算H2sub>+sup>的结构参数

陈景

《中国工程科学》 2004年第6卷第11期页码 29-32

摘要：

对氢分子离子提出了氢原子质子化的结构模型，从微观时标和宏观时标分析了H2sub>+sup>中库仑吸引力和两核排斥力的动态平衡，认为氢原子畸变后的电子云在两核中点产生e/8的电荷重心时可以束缚住一个裸质子；据此推导出键长、键能及力常数的计算公式；使用原子单位分别获得Resub>=2 au，Desub>=0.109 735 au，k=0.109

关键词：氢分子离子键长键能力常数

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Deciphering the effect of sodium dodecylbenzene sulfonate on up-flow anaerobic sludge blanket treatment of synthetic sulfate-containing wastewater

《环境科学与工程前沿（英文）》 2021年第15卷第5期 doi: 10.1007/s11783-020-1385-z

摘要：

• UASB reactor can work efficiently with high COD/SO₄²^- ratios when SDBS exists.

关键词： Up-flow anaerobic sludge blanket Organic sulfur Sodium dodecylbenzene sulfonate COD/SO₄²⁻ ratio Microbial community

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Performance and mechanism of carbamazepine removal by FeS-SO process: experimental investigation and DFT calculations

《环境科学与工程前沿（英文）》 2023年第17卷第9期 doi: 10.1007/s11783-023-1713-1

摘要：

● Synergistic removal of carbamazepine (CBZ) was obtained in the FeS-S₂O₈^2– process.

关键词： FeS S₂O₈^2– Carbamazepine DFT calculations Degradation routes

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Facile synthesis and enhanced visible-light photocatalytic activity of Ti

Xiaojie Zhang,Lei Wang,Shuqing Chen,Yi Huang,Zhuonan Song,Miao Yu

《化学科学与工程前沿（英文）》 2015年第9卷第3期页码 349-358 doi: 10.1007/s11705-015-1523-5

摘要： Ti -doped TiO nanosheets with tunable phase composition (doped TiO (A/R)) were synthesized via a hydrothermal method with high surface area anatase TiO nanosheets TiO (A) as a substrate, structure directing agent, and inhibitor; the activity was evaluated using a probe reaction-photocatalytic CO conversion to methane under visible light irradiation with H as an electron donor and hydrogen source. High-resolution transmission electron microscope (HRTEM), field emission scanning electron microscope, UV-Vis diffuse reflectance spectra, and X-ray diffraction (XRD) etc., were used to characterize the photocatalysts. XRD and HRTEM measurements confirmed the existence of anatase-rutile phase junction, while Ti and single-electron-trapped oxygen vacancy in the doped TiO (A/R) photocatalyst were revealed byelectron paramagnetic resonance (EPR) measurements. Effects of hydrothermal synthesis temperature and the amount of added anatase TiO on the photocatalytic activity were elucidated. Significantly enhanced photocatalytic activity of doped TiO (A/R) was observed; under the optimized synthesis conditions, CH generation rate of doped TiO (A/R) was 2.3 times that of Ti -doped rutile TiO .

关键词： Ti³⁺-doped TiO₂ photocatalytic CO₂ conversion visible light irradiation

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配位不饱和Au-O-Ti3+sup>活性位点的构建及其在低温丙烯气相环氧化反应中强化氢气效率的研究 Article

宋钊宁, 闫昊, 袁俊聪, 马宏飞, 曹建琳, 王永祥, 王强, 彭冲, 邓风, 冯翔, 陈德, 杨朝合, 胡永康

《工程（英文）》 2023年第25卷第6期页码 144-156 doi: 10.1016/j.eng.2023.01.008

摘要：

自1998年以来，人们广泛认为Au/Ti基催化剂的Au-O-Ti4+sup>位点是在相对高温条件下丙烯气相环氧化反应的活性位点，但该类催化剂的H2sub>有效利用率普遍较低本工作通过调整处理后S-1晶种中Si-OH和Bu3sub>NH+sup>的量，定量构建了Au-O-Ti3+sup>活性位点。4+sup>活性位点上的明显增高。此外，氨程序升温脱附（NH3sub>-TPD）和X射线光电子能谱（XPS）表征以及密度泛函数理论（DFT）计算表明，在相对低温条件下，Au-O-Ti3+sup>活性位点中配位不饱和Ti3+sup>位点促进了Au和Ti3+sup>之间的电子转移，从而增强了催化剂对O2sub>的吸附能力，有效促进H2sub>O2sub

关键词：丙烯环氧化 H2sub>有效利用率 Au/Ti双功能催化剂配位不饱和Ti位点密度泛函理论

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Effects of ancillary ligands in acceptorless benzyl alcohol dehydrogenation mediated by phosphine-free cobalt complexes

《化学科学与工程前沿（英文）》 2023年第17卷第3期页码 314-325 doi: 10.1007/s11705-022-2219-2

摘要： Acceptorless alcohol dehydrogenation stands out as one of the most promising strategies in hydrogen storage technologies. Among various catalytic systems for this reaction, cost-effective molecular catalysts using phosphine-free ligands have gained considerable attention. However, the central challenge for using non-precious metals is to overcome the propensity of reacting by one-electron pathway. Herein, we synthesized a phosphine-free η⁵-C₅Me₅-Co complex by using the metal–ligand cooperative strategy and compared its activity with analogous catalysts toward acceptorless alcohol dehydrogenation. The catalyst showed excellent performance with a turnover number of 130.4 and a selectivity close to 100%. The improved performance among the class of η⁵-C₅Me₅-Co complexes could be attributed to the more accessible Co center and its cooperation with the redox-active ligand. To further study the systematic structure-activity relationship, we investigated the electronic structures of η⁵-C₅Me₅-Co complexes by a set of characterizations. The results showed that the redox-active ligand has a significant influence on the η⁵-C₅Me₅-Co moiety. In the meantime, the proximal O⁻/OH group is beneficial for shuttling protons. For the catalytic cycle, two dehydrogenation scenarios were interrogated through density functional theory, and the result suggested that the outer-sphere pathway was preferred. The formation of a dihydrogen complex was the rate-determining step with a ΔG value of 16.9 kcal∙mol^‒1. The electron population demonstrated that the η⁵-C₅Me₅ ligand played a key role in stabilizing transition states during dehydrogenation steps. This work identified the roles of vital ligand components to boost catalytic performance and offered rationales for designing metal–ligand cooperative nonprecious metal complexes.

关键词： acceptorless alcohol dehydrogenation η⁵-C₅Me₅-Co metal–ligand cooperation theoretical calculation

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An electrochemical process that uses an Fe

Chaojie Jiang, Lifen Liu, John C. Crittenden

《环境科学与工程前沿（英文）》 2016年第10卷第4期 doi: 10.1007/s11783-016-0860-z

摘要： A bio-electrochemical fuel cell reactor with cathodic Fe /TiO generates electricity. It destroys recalcitrant pollutants in cathode chamber without photocatalysis. Fe /TiO generates reactive oxygenated species in the dark or under photocatalysis. Cathodic produced ROS (hydroxy radical/superoxide radical) can degrade tetracycline or dyes. Electricity generation is enhanced by semiconductor catalyzed cathodic degradation of pollutants. In this study, a new water treatment system that couples (photo-) electrochemical catalysis (PEC or EC) in a microbial fuel cell (MFC) was configured using a stainless-steel (SS) cathode coated with Fe /TiO . We examined the destruction of methylene blue (MB) and tetracycline. Fe /TiO was prepared using a chemical reduction-deposition method and coated onto an SS wire mesh (500 mesh) using a sol technique. The anode generates electricity using microbes (bio-anode). Connected via wire and ohmic resistance, the system requires a short reaction time and operates at a low cost by effectively removing 94% MB (initial concentration 20 mg·L ) and 83% TOC/TOC under visible light illumination (50 W; 1.99 mW·cm for 120 min, MFC-PEC). The removal was similar even without light irradiation (MFC-EC). The of the MFC-PEC system was approximately 0.675 kWh·m ·order , whereas that of the MFC-EC system was zero. The system was able to remove 70% COD in tetracycline solution (initial tetracycline concentration 100 mg·L ) after 120 min of visible light illumination; without light, the removal was 15% lower. The destruction of MB and tetracycline in both traditional photocatalysis and photoelectrocatalysis systems was notably low. The electron spin-resonance spectroscopy (ESR) study demonstrated that ·OH was formed under visible light, and ·O was formed without light. The bio-electricity-activated O and ROS (reactive oxidizing species) generation by Fe /TiO effectively degraded the pollutants. This cathodic degradation improved the electricity generation by accepting and consuming more electrons from the bio-anode.

关键词： Bio-anode Photocatalytic cathode Fe⁰/TiO₂ ESR Dye and antibiotics Advanced oxidation

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Fabrication of three-dimensional porous La-doped SrTiO3 microspheres with enhanced visible light catalytic

Dong Yang, Xiaoyan Zou, Yuanyuan Sun, Zhenwei Tong, Zhongyi Jiang

《化学科学与工程前沿（英文）》 2018年第12卷第3期页码 440-449 doi: 10.1007/s11705-018-1700-4

摘要：

In recent years, much effort has been focused on the development of the photocatalysts with high performance under visible light irradiation. In this paper, three-dimensional porous La-doped SrTiO₃ (LST) microspheres were prepared by a modified sol–gel method, in which the agarose gel/SrCO₃ microsphere and La₂O₃ were employed as the template and the La resource, respectively. The as-prepared LST microspheres exhibit a porous structure with a diameter of about 10 µm and a surface pore size of about 100 nm. The La element was doped into the crystal lattice of SrTiO₃ by the substitution of La³⁺ for Sr²⁺. Therefore, the absorption edge of LST samples shifts toward the visible light region, and their photocatalytic activity for the Cr(VI) reduction is enhanced under visible light. Among all LST samples, LST-0.5 (the La³⁺ doping content is 0.5 wt-%) exhibited the highest visible-light photocatalytic activity, which can reduce 84% Cr(VI) within 100 min. This LST materials may become a promising photocatalyst for the facile treatment of wastewater containing poisonous heavy metal ions.

关键词： SrTiO₃ La³⁺ doping porous microsphere visible-light photocatalysis Cr(VI) reduction

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五唑阴离子——前行中的新一代高含能材料

林秋汉, 王鹏程, 许元刚, 陆明

《工程（英文）》 2020年第6卷第9期页码 964-966 doi: 10.1016/j.eng.2020.04.011

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different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH3sub>

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要： Three kinds of Ce-based catalysts (CePO₄, CeVO₄, Ce₂(SO₄)₃) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH₃. NH₃-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO₄ > CeVO₄ > Ce₂(SO₄)₃, which is in agreement with their abilities of NH₃ adsorption capacities. The highest NO conversion rate of CePO₄ could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO₄^3–, VO₄^3– and SO₄^2– on NH₃-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH₃ temperature programmed desorption, H₂ temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce⁴⁺, large NH₃ adsorption capacity, high and early H₂ consumptions, and suitable microstructures for gas adsorption. Finally, CePO₄ and CeVO₄ catalysts also exhibited relatively strong tolerance of SO₂, and the upward trend about 8% was detected due to the sulfation enhancement by SO₂ for Ce₂(SO₄)₃.

关键词： CePO₄ CeVO₄ Ce₂(SO₄)₃ selective catalytic reduction NO removal