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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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用高光谱发光法研究Cu(In<sub><i>xi>sub>,Ga<sub>1–<i>xi>sub>)Se<sub>2sub> (CIGS)模块中由P1引起的功率损耗的成因 Article

César Omar Ramírez Quiroz, Laura-Isabelle Dion-Bertrand, Christoph J. Brabec, Joachim Müller, Kay Orgassa

《工程（英文）》 2020年 第6卷 第12期   页码 1395-1402 doi: 10.1016/j.eng.2019.12.019

摘要：

在本文中，我们利用了高光谱高分辨率光致发光映射技术，这是一个强大的工具，可用于选择和优化在Cu(In<sub>xsub>,Ga<sub>1-xsub>)Se<sub>2sub>（CIGS）模块上对子电池进行图案化互连的激光烧蚀工艺。

关键词： Cu(Inx     Ga1–x)Se2     电池到模块的效率差距     由P1引起的功率损耗     高光谱光致发光     激光烧蚀短程热效应    

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Simultaneous removal of NO and chlorobenzene on VO/TiO granular catalyst: Kinetic study and performance

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1363-5

摘要：

• A V2O5/TiO2 granular catalyst for simultaneous removal of NO and chlorobenzene.

关键词： NOx     Chlorobenzene     Simultaneous removal     Kinetic study     Performance prediction     V2O5/TiO2     Graphical abstract    

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NO<sub><i>xi>sub> and H<sub>2sub>S formation in the reductive zone of air-staged combustion of

Jinzhi CAI, Dan LI, Denggao CHEN, Zhenshan LI

《能源前沿（英文）》 2021年 第15卷 第1期   页码 4-13 doi: 10.1007/s11708-020-0804-y

摘要： Low NO combustion of blended coals is widely used in coal-fired boilers in China to control NO emission; thus, it is necessary to understand the formation mechanism of NO and H S during the combustion of blended coals. This paper focused on the investigation of reductive gases in the formation of NO and H S in the reductive zone of blended coals during combustion. Experiments with Zhundong (ZD) and Commercial (GE) coal and their blends with different mixing ratios were conducted in a drop tube furnace at 1200°C–1400°C with an excessive air ratio of 0.6–1.2. The coal conversion and formation characteristics of CO, H S, and NO in the fuel-rich zone were carefully studied under different experimental conditions for different blend ratios. Blending ZD into GE was found to increase not only the coal conversion but also the concentrations of CO and H S as NO reduction accelerated. Both the CO and H S concentrations inblended coal combustion increase with an increase in the combustion temperature and a decrease in the excessive air ratio. Based on accumulated experimental data, one interesting finding was that NO and H S from blended coal combustion were almost directly dependent on the CO concentration, and the CO concentration of the blended coal combustion depended on the single char gasification conversion.Thus, CO, NO , and H S formation characteristics from blended coal combustion can be well predicted by single char gasification kinetics.

关键词： blended coal combustion     NOx formation     H2S formation     air staged combustion    

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H<sub>2sub> 对Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub> 催化剂NO<sub><i>xi>sub> 存储和还原机理的影响研究 Article

王攀, 裔静, 孙川, 罗鹏, 雷利利

《工程（英文）》 2019年 第5卷 第3期   页码 568-575 doi: 10.1016/j.eng.2019.02.005

摘要：

本研究采用浸渍法制备了Pt-Ba-Ce/γ-Al<sub>2sub>O<sub>3sub>催化剂，利用实验评价了H<sub>2sub> 对NSR（NO<sub>x<结果表明，透射电子显微镜（TEM）显示X 射线衍射（XRD）光谱中观察到的PtO<sub>xsub>、CeO<sub>2sub> 和BaCO<sub>3sub> 峰很好地分散在在NO<sub>xsub> 完全存储- 还原实验中，NO<sub>2sub> 产量的增加使NO<sub>xsub> 的存储能力在250~350 ℃ 的温度范围内大大提高在NO<sub>xsub> 吸附和脱附循环实验中，随着H<sub>2sub>暴露时间（30 s、45 s 和60 s）延长，NO<sub>xsub> 的存储效率和转化率增加适当增加H<sub>2sub>量加速了硝酸盐或亚硝酸盐的分解，有利于NO<sub>xsub> 存储-还原，并促进了下一循环NSR吸附位点的再生。

关键词： Pt–Ba–Ce/γ-Al<sub>2sub>O<sub>3sub> 催化剂，物理化学性质，NO<sub><i>xi>sub>存储和还原，NO<sub><i>xi>sub> 排放，H<sub>2sub> 还原剂    

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><i>In situi> growth of phosphorized ZIF-67-derived amorphous CoP/Cu<sub>2sub>O@CF electrocatalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1430-1439 doi: 10.1007/s11705-023-2320-1

摘要： Transition metal phosphides have been extensively studied for catalytic applications in water splitting. Herein, we report an in situ phosphorization of zeolitic imidazole frameworks (ZIF-67) to generate amorphous cobalt phosphide/ZIF-67 heterojunction on a self-supporting copper foam (CF) substrate with excellent performance for hydrogen evolution reaction (HER). The needle-leaf like copper hydroxide was anchored on CF surface, which acted as implantation to grow ZIF-67. The intermediate product was phosphorized to obtain final electrocatalyst (CoP/Cu2O@CF) with uniform particle size, exhibiting a rhombic dodecahedron structure with wrinkles on the surface. The electrochemical measurement proved that CoP/Cu2O@CF catalyst exhibited excellent HER activity and long-term stability in 1.0 mol·L–1 KOH solution. The overpotential was only 62 mV with the Tafel slope of 83 mV·dec–1 at a current density of 10 mA·cm–2, with a large electrochemical active surface area. It also showed competitive performance at large current which indicated the potential application to industrial water electrolysis to produce hydrogen. First-principle calculations illustrated that benefit from the construction of CoP/ZIF-67 heterojunction, the d-band center of CoP downshifted after bonding with ZIF-67 and the Gibbs free energy (ΔGH*) changed from –0.18 to –0.11 eV, confirming both decrease in overpotential and excellent HER activity. This work illustrates the efficient HER activity of CoP/Cu2O@CF catalyst, which will act as a potential candidate for precious metal electrocatalysts.

关键词： CoP/Cu2O@CF     electrocatalyst     phosphorization     HER     DFT    

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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年 第15卷 第3期   页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO2) composite (TiN/N-TiO2) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO2 and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO2 composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO2 and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO2 with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO2 composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H2 evolution     TiN/N-TiO2 composite     plasmonic effect     in-situ nitridation    

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Photosynthesis and related metabolic mechanism of promoted rice (<i>Oryza sativai> L.) growth by TiO<sub>2sub> nanoparticles

Yingdan Zhang, Na Liu, Wei Wang, Jianteng Sun, Lizhong Zhu

《环境科学与工程前沿（英文）》 2020年 第14卷 第6期 doi: 10.1007/s11783-020-1282-5

摘要： Abstract • The rice growth was promoted by nano-TiO2 of 0.1–100 mg/L. • Nano-TiO2 enhanced the energy storage in photosynthesis. • Nano-TiO2 reduced energy consumption in carbohydrate metabolism and TCA cycle. Titanium dioxide nanoparticle (nano-TiO2), as an excellent UV absorbent and photo-catalyst, has been widely applied in modern industry, thus inevitably discharged into environment. We proposed that nano-TiO2 in soil can promote crop yield through photosynthetic and metabolic disturbance, therefore, we investigated the effects of nano-TiO2 exposure on related physiologic-biochemical properties of rice (Oryza sativa L.). Results showed that rice biomass was increased >30% at every applied dosage (0.1–100 mg/L) of nano-TiO2. The actual photosynthetic rate (Y(II)) significantly increased by 10.0% and 17.2% in the treatments of 10 and 100 mg/L respectively, indicating an increased energy production from photosynthesis. Besides, non-photochemical quenching (Y(NPQ)) significantly decreased by 19.8%–26.0% of the control in all treatments respectively, representing a decline in heat dissipation. Detailed metabolism fingerprinting further revealed that a fortified transformation of monosaccharides (D-fructose, D-galactose, and D-talose) to disaccharides (D-cellobiose, and D-lactose) was accompanied with a weakened citric acid cycle, confirming the decrease of energy consumption in metabolism. All these results elucidated that nano-TiO2 promoted rice growth through the upregulation of energy storage in photosynthesis and the downregulation of energy consumption in metabolism. This study provides a mechanistic understanding of the stress-response hormesis of rice after exposure to nano-TiO2, and provides worthy information on the potential application and risk of nanomaterials in agricultural production.

关键词： Nano-TiO2     Rice     Photosynthesis     Metabolomics     Energy storage    

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NiFeRuO<sub><i>xi>sub> nanosheets on Ni foam as an electrocatalyst for efficient

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1698-1706 doi: 10.1007/s11705-023-2334-8

摘要： The electrocatalyst NiFeRuOx/NF, comprised of NiFeRuOx nanosheets grown on Ni foam, was synthesized using a hydrothermal process followed by thermal annealing. NiFeRuOx/NF displays high electrocatalytic activity and stability for overall alkaline seawater splitting: 98 mV@ 10 mA∙cm−2 in hydrogen evolution reaction, 318 mV@ 50 mA∙cm−2 in oxygen evolution reaction, and a cell voltage of 1.53 V@ 10 mA∙cm−2, as well as 20 h of durability. A solar-driven system containing such a bifunctional NiFeRuOx/NF has an almost 100% Faradaic efficiency. The NiFeRuOx coating around Ni foam is an anti-corrosion layer and also a critical factor for enhancement of bifunctional performances.

关键词： NiFeRuOx nanosheets     Ni foam     electrocatalysis     overall seawater splitting     solar-driven system    

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Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11684-022-1565-0

摘要：

● Cu addition enhances CH3OH oxidation and alleviates its inhibitory effect on SCR.

关键词： Copper modification     Sb-CeZr2Ox catalyst     NOx     Methanol     Simultaneous removal    

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Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 525-535 doi: 10.1007/s11705-022-2232-5

摘要： Fe–Nx nanoparticles-embedded porous carbons with a desirable superstructure have attracted immense attention as promising catalysts for electrochemical oxygen reduction reaction. Herein, we employed Fe-coordinated covalent triazine polymer for the fabrication of Fe–Nx nanoparticle-embedded porous carbon nanoflorets (Fe/N@CNFs) employing a hypersaline-confinement-conversion strategy. Presence of tailored N types within the covalent triazine polymer interwork in high proportions contributes to the generation of Fe/N coordination and subsequent Fe–Nx nanoparticles. Owing to the utilization of NaCl crystals, the resultant Fe/N@CNF-800 which was generated by pyrolysis at 800 °C showed nanoflower structure and large specific surface area, which remarkably suppressed the agglomeration of high catalytic active sites. As expect, the Fe/N@CNF-800 exhibited unexpected oxygen reduction reaction catalytic performance with an ultrahigh half-wave potential (0.89 V vs. reversible hydrogen electrode), a dominant 4e– transfer approach and great cycle stability (> 92% after 100000 s). As a demonstration, the Fe/N-PCNF-800-assembled zinc–air battery delivered a high open circuit voltage of 1.51 V, a maximum peak power density of 164 mW·cm–2, as well as eminent rate performance, surpassing those of commercial Pt/C. This contribution offers a valuable avenue to exploit efficient metal nanoparticles-based carbon catalysts towards energy-related electrocatalytic reactions and beyond.

关键词： Fe–Nx nanoparticles     hypersaline-confinement conversion     floret-like carbon     covalent triazine polymers     oxygen reduction reaction    

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Advantageous mechanochemical synthesis of copper(I) selenide semiconductor, characterization, and properties

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 433-442 doi: 10.1007/s11705-021-2066-6

摘要： Copper(I) selenide-nanocrystalline semiconductor was synthesized via one-step mechanochemical synthesis after 5 min milling in a planetary ball mill. The kinetics of synthesis was followed by X-ray powder diffraction analysis and specific surface area measurements of milled 2Cu/Se mixtures. The X-ray diffraction confirmed the orthorhombic crystal structure of Cu2Se with the crystallite size ~25 nm. The surface chemical structure was studied by X-ray photoelectron spectroscopy, whereby the binding energy of the Cu 2p and Se 3d signals corresponded to Cu+ and Se2– oxidation states. Transmission electron microscopy revealed agglomerated nanocrystals and confirmed their orthorhombic structure, as well. The optical properties were studied utilizing ultraviolet-visible spectroscopy and photoluminescence spectroscopy. The direct bandgap energy 3.7 eV indicated a blue-shift phenomenon due to the quantum size effect. This type of Cu2Se synthesis can be easily adapted to production dimensions using an industrial vibratory mill. The advantages of mechanochemical synthesis represent the potential for inexpensive, environmentally-friendly, and waste-free manufacturing of Cu2Se.

关键词： Cu2Se     berzelianite     nanocrystalline semiconductor     mechanochemical synthesis     planetary ball mill    

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CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction mechanistic study

《环境科学与工程前沿（英文）》 2022年 第16卷 第5期 doi: 10.1007/s11783-022-1539-2

摘要：

• CeO2 doping significantly improved low-temperature NH3-SCR activity on FeTiOx.

关键词： NH3-SCR     CeO2 doping     Low-temperature NOx removal     Improved redox property     In situ XAFS analysis    

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photocatalytic performance through the evolution of the properties due to the phase transition from NaBiO·2HO

《能源前沿（英文）》 2022年 第16卷 第3期   页码 471-482 doi: 10.1007/s11708-021-0778-4

摘要： The phase transition process of a photocatalytic system from NaBiO3·2H2O to BiO2–x has been investigated to understand the important factors that affect photocatalytic performance in a composite system. It is found that a proper amount of BiO2–x on the surface of NaBiO3·2H2O could effectively suppress the electron/hole recombination and increase the exposed reactive sites for photocatalytic reaction. A fully covered BiO2–x on NaBiO3·2H2O results in a dramatical decrease of photocatalytic degradation of dye. An over long hydrothermal process can result in BiO2–x with reduced oxygen vacancies, which degrades the photocatalytic activity. Furthermore, the photocatalytic reduction ability of CO2 conversion has been investigated, indicating that the surface activity to different reactants also directly affects the catalytic performance. The investigation of the gradient phase transition process presents a clear guidance to construct a desired photocatalytic system, in addition to selecting gradient materials with suitable bandgap structure and a morphology with different fraction and distribution of each component. The defect evolution of each component during construction of a composite is also an important factor that should be optimized and considered in making a composite to achieve high photocatalytic efficiency.

关键词： composite construction     distribution     BiO2–x     evolution of defects    

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Effects of Pd doping on N

Mingxin Dong, Jun Wang, Jinxin Zhu, Jianqiang Wang, Wulin Wang, Meiqing Shen

《环境科学与工程前沿（英文）》 2017年 第11卷 第6期 doi: 10.1007/s11783-017-0976-9

摘要： N O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N O formation over Pt/BaO/Al O catalyst. Three types of catalysts, Pt/BaO/Al O , Pt/Pd mechanical mixing catalyst (Pt/BaO/Al O +Pd/Al O ) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al O ) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H /CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H -TPR techniques. In addition, temperature programmed reactions of NO with H /CO were conducted to obtain further information about N O formation mechanism. Compared with Pt/BaO/Al O , (Pt/BaO/Al O +Pd/Al O ) produced less N O and more NH during NO storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al O +Al O ). Temperature programmed reactions of NO with H /CO results showed that Pd/Al O component in (Pt/BaO/Al O +Pd/Al O ) played an important role in NO reduction to NH , and the formed NH could reduce NO to N leading to a decrease in N O formation. Most of N O formed over (Pt-Pd/BaO/Al O +Al O ) was originated from Pd/BaO/Al O component. H -TPR results indicated Pd-Ba interaction resulted in more difficult-to-reduce PdO species over Pd/BaO/Al O , which inhibits the NO dissociation and thus drives the selectivity to N O in NO reduction.

关键词： NOx storage reduction     Pt/BaO/Al2O3     Pd doping     N2O formation     Optimization    

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标题 作者 时间 类型 操作

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

期刊论文

用高光谱发光法研究Cu(In<sub><i>xi>sub>,Ga<sub>1–<i>xi>sub>)Se<sub>2sub> (CIGS)模块中由P1引起的功率损耗的成因

César Omar Ramírez Quiroz, Laura-Isabelle Dion-Bertrand, Christoph J. Brabec, Joachim Müller, Kay Orgassa

期刊论文

Simultaneous removal of NO and chlorobenzene on VO/TiO granular catalyst: Kinetic study and performance

期刊论文

NO<sub><i>xi>sub> and H<sub>2sub>S formation in the reductive zone of air-staged combustion of

Jinzhi CAI, Dan LI, Denggao CHEN, Zhenshan LI

期刊论文

H<sub>2sub> 对Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub> 催化剂NO<sub><i>xi>sub> 存储和还原机理的影响研究

王攀, 裔静, 孙川, 罗鹏, 雷利利

期刊论文

><i>In situi> growth of phosphorized ZIF-67-derived amorphous CoP/Cu<sub>2sub>O@CF electrocatalyst

期刊论文

grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

期刊论文

Photosynthesis and related metabolic mechanism of promoted rice (<i>Oryza sativai> L.) growth by TiO<sub>2sub> nanoparticles

Yingdan Zhang, Na Liu, Wei Wang, Jianteng Sun, Lizhong Zhu

期刊论文

NiFeRuO<sub><i>xi>sub> nanosheets on Ni foam as an electrocatalyst for efficient

期刊论文

Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

期刊论文

Floret-like Fe–N nanoparticle-embedded porous carbon superstructures from a Fe-covalent triazine polymer

期刊论文

Advantageous mechanochemical synthesis of copper(I) selenide semiconductor, characterization, and properties

期刊论文

CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction mechanistic study

期刊论文

photocatalytic performance through the evolution of the properties due to the phase transition from NaBiO·2HO

期刊论文

Effects of Pd doping on N

Mingxin Dong, Jun Wang, Jinxin Zhu, Jianqiang Wang, Wulin Wang, Meiqing Shen

期刊论文