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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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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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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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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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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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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>)>sp sub>= 265.3 s）均稍优于六硝基六氮杂异伍兹烷（CL-20：Q = 6.23 kJ·g‒1sup>，I<sub

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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Application of Fe

Xiaowei ZHANG,Qinyan YUE,Dongting YUE,Baoyu GAO,Xiaojuan WANG

《环境科学与工程前沿（英文）》 2015年第9卷第3期页码 402-410 doi: 10.1007/s11783-014-0659-8

摘要： Dyes are common pollutants in textile wastewaters, and the treatment of the wastewater has now attracted much attention due to its wide application and low biodegradability. In this study, Fe /C/Clay ceramics, a kind of novel micro-electrolysis filler, were sintered and employed in a dynamic micro-electrolysis reactor for synthetic Acid Red 73 (AR73) and Reactive Blue 4 (RB4) wastewater treatment. The effects of influent pH, hydraulic retention time (HRT), and aeration on the decoloration efficiencies of AR73 and RB4 were studied. The optimum conditions for wastewater treatment were: AR73, influent pH of 4, HRT of 2 h and aeration; RB4, influent pH of 5, HRT of 6 h and aeration. Under the optimum conditions, decoloration efficiency of AR73 and RB4 wastewater was 96% and 83%, respectively. Results of UV-vis spectrum scanning demonstrated that the chromophores were broken. Continuous running tests showed that improvement of micro-electrolysis system with Fe /C/Clay ceramics for AR73 and RB4 synthetic wastewater treatment could avoid failure of micro-electrolysis reactor, which indicated great potential for the practical application of the ceramics in the field of actual industrial wastewater treatment.

关键词： Fe⁰/C/Clay ceramics micro-electrolysis Acid Red 73 Reactive Blue 4 synthetic wastewater

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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值得注意的是，该活性位点主导反应时，最佳温度可从200 °C显著降低至138 °C，并使催化剂保持前所未有的43.6%的H2sub>有效利用率、90.7%的环氧丙烷（PO）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。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本工作所报道的结果为强化丙烯直接气相环氧化反应的H2sub>有效利用率提供了新的思路，而且为低温下丙烯直接气相环氧化反应的工业化推进开辟了新的机会。

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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NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

《化学科学与工程前沿（英文）》 2023年第17卷第12期页码 1973-1985 doi: 10.1007/s11705-023-2364-2

摘要： Ammonia is crucial in industry and agriculture, but its production is hindered by environmental concerns and energy-intensive processes. Hence, developing an efficient and environmentally friendly catalyst is imperative. In this study, we employed a straightforward and efficient impregnation technique to create various Cu-doped catalysts. Notably, the optimized 10Fe-8Cu/TiO₂ catalyst exhibited exceptional catalytic performance in converting NO to NH₃, achieving an NO conversion rate exceeding 80% and an NH₃ selectivity exceeding 98% at atmospheric pressure and 350 °C. We employed in situ diffuse reflectance Fourier transform infrared spectroscopy and conducted density functional theory calculations to investigate the intermediates and subsequent adsorption. Our findings unequivocally demonstrate that Cu doping enhances the rate-limiting hydrogenation step and lowers the energy barrier for NH₃ desorption, thereby resulting in improved NO conversion and enhanced selectivity toward ammonia. This study presents a pioneering approach toward energy-efficient ammonia synthesis and recycling of nitrogen sources.

关键词： NO hydrogenation synthetic ammonia 10Fe-xCu/TiO₂ high selectivity

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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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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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Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

《能源前沿（英文）》 2021年第15卷第3期页码 732-743 doi: 10.1007/s11708-021-0772-x

摘要： In this study, the electronic and photocatalytic properties of core-shell heterojunctions photocatalysts with reversible configuration of TiO₂ and Bi₂O₃ layers were studied. The core-shell nanostructure, obtained by efficient control of the sol-gel polymerization and impregnation method of variable precursors of semiconductors, makes it possible to study selectively the role of the interfacial charge transfer in each configuration. The morphological, optical, and chemical composition of the core-shell nanostructures were characterized by high-resolution transmission electron microscopy, UV-visible spectroscopy and X-ray photoelectron spectroscopy. The results show the formation of homogenous TiO₂ anatase and Bi₂O₃ layers with a thickness of around 10 and 8 nm, respectively. The interfacial charge carrier dynamic was tracked using time resolved microwave conductivity and transition photocurrent density. The charge transfer, their density, and lifetime were found to rely on the layout layers in the core-shell nanostructure. In optimal core-shell design, Bi₂O₃ collects holes from TiO₂, leaving electrons free to react and increase by 5 times the photocatalytic efficiency toward H₂ generation. This study provides new insight into the importance of the design and elaboration of optimal heterojunction based on the photocatalyst system to improve the photocatalytic activity.

关键词： photocatalysis core-shell heterojunction H₂ TiO₂ Bi₂O₃

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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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Inexpensive synthesis of a high-performance Fe

Nadir Abbas, Godlisten N. Shao, Syed M. Imran, Muhammad S. Haider, Hee Taik Kim

《化学科学与工程前沿（英文）》 2016年第10卷第3期页码 405-416 doi: 10.1007/s11705-016-1579-x

摘要： A sol-gel technique has been developed for the synthesis of a magnetite-silica-titania (Fe O -SiO -TiO ) tertiary nanocomposite with improved photocatalytic properties based on the use of inexpensive titania and silica precursors. The exceptional photocatalytic activity of the resulting materials was demonstrated by using them to photocatalyze the degradation of methylene blue solution. The best formulation achieved 98% methylene blue degradation. An interesting feature of the present work was the ability to magnetically separate and reuse the catalyst. The efficiency of the catalyst remained high during two reuses. The synthesized nanomaterials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared (FTIR) spectroscopy, ultra-violet-visible spectroscopy, diffuse reflectance spectroscopy, and thermogravimetric analysis. XRD analysis revealed the formation of multicrystalline systems of cubic magnetite and anatase titania crystals. SEM and TEM characterization revealed well-developed and homogeneously dispersed particles of size less than 15 nm. FTIR spectra confirmed the chemical interaction of titania and silica. It was further noticed that the optical properties of the prepared materials were dependent on the relative contents of their constituent metal oxides.

关键词： sol-gel photocatalysis magnetic recovery TiO₂ Fe₃O₄ SiO₂