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Graphene-like -BN supported polyhedral NiS/NiS nanocrystals with excellent photocatalytic performance

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1537-1549 doi: 10.1007/s11705-021-2094-2

摘要： Human health is deteriorating due to the effluent containing heavy metal ions and organic dyes. Hence, photoreduction of Cr(VI) to Cr(III) and degradation of rhodamine B (RhB) using a novel photocatalyst is particularly important. In this work, h-BN/NiS2/NiS composites were prepared via a simple solvothermal method and a double Z-scheme heterojunction was constructed for efficiently removing RhB and Cr(VI). The 7 wt-% h-BN/NiS2/NiS composites were characterized via a larger specific surface area (15.12 m2·g–1), stronger light absorption capacity, excellent chemical stability, and high yield of electrons and holes. The experimental result indicated that the photoreduction efficiency of the 7 wt-% h-BN/NiS2/NiS photocatalyst achieved 98.5% for Cr(VI) after 120 min, which was about 3 times higher than that of NiS2/NiS (34%). However, the removal rate of RhB by the 7 wt-% h-BN/NiS2/NiS photocatalyst reached 80%. This is due to the double Z-scheme heterojunction formed between NiS2/NiS and h-BN, which improved the charge separation efficiency and transmission efficiency. Besides, the influence of diverse photogenerated electron and hole scavengers upon the photoreduction of Cr(VI) was studied, the results indicated that graphene-like h-BN promoted transportation of photoinduced charges on the surface of the h-BN/NiS2/NiS photocatalyst via the interfacial effects.

关键词： graphene-like h-BN     h-BN/NiS2/NiS composites     photocatalysis     Cr(VI) reduction     degradation of RhB    

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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>xsub> storage and reduction）催化剂存储和还原机理的影响，并采用综合表征技术研究了Pt-Ba-Ce /γ-Al<sub>2sub>O<sub>3sub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> 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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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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<i>Ni>-Positive ion activated rapid addition and mitochondrial targeting ratiometric fluorescent probesfor <i>in vivoi> cell H<sub>2sub>S imaging

Yan Shi, Fangjun Huo, Yongkang Yue, Caixia Yin

《化学科学与工程前沿（英文）》 2022年 第16卷 第1期   页码 64-71 doi: 10.1007/s11705-021-2048-8

摘要： Heterocyclic compound quinoline and its derivatives exist in natural compounds and have a broad spectrum of biological activity. They play an important role in the design of new structural entities for medical applications. Similarly, indoles and their derivatives are found widely in nature. Amino acids, alkaloids and auxin are all derivatives of indoles, as are dyes, and their condensation with aldehydes makes it easy to construct reaction sites for nucleophilic addition agents. In this work, we combine these two groups organically to construct a rapid response site (within 30 s) for H S, and at the same time, a ratiometric fluorescence response is presented throughout the process of H S detection. As such, the lower detection limit can reach 55.7 nmol/L for H S. In addition, cell imaging shows that this probe can be used for the mitochondrial targeted detection of endogenous and exogenous H S. Finally, this probe application was verified by imaging H S in nude mice.

关键词： heterocyclic compound     hydrogen sulfide     ratiometric     mitochondrial targeted    

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High specificity detection of Pb

Ruozhen YU,Zheng FANG,Wei MENG,Zhenguang YAN,Lina DU,Hong WANG,Zhengtao LIU

《环境科学与工程前沿（英文）》 2014年 第8卷 第5期   页码 729-736 doi: 10.1007/s11783-013-0611-3

摘要： Only one bifunctional metal-chelator was used to prepare immunogen and coating antigen in all of the previous researches. However, the antibody-specific recognition to the spacer arm of the bifunctional metal-chelator might lower the specificity of heavy metal ions immunoassay. Two different bifunctional metal-chelators were adopted to prepare the immunogen and coating antigen respectively in our study to avoid this problem. The conjugates of keyhole limpet hemocyanin (KLH) and -SCN-Bz-DTPA-Pb were used as immunogen, whereas the conjugates of bovine serum albumin (BSA) and -NH -Bn-DTPA-Pb were used as coating antigen. Polyclonal antibodies specific to DTPA-Pb chelates were obtained from rabbits. Indirect competitive enzyme-linked immunosorbent assay (ELISA) was adopted to detect Pb ion solutions prepared by Pb standard solution and ultrapure water. In the mixing microplate, DTPA and Pb ions formed chelates and combined with specific antibodies. After incubation, the DTPA-Pb and the antibodies complex were added into the wells of the reaction microplate. The reaction microplate was coated by the conjugates of BSA and -NH -DTPA-Pb, which competed for the specific antibodies. The result signals presented a good sigmoid curve when the Pb concentration ranges from 0.01 to 100 mg·L . The IC50 of the indirect competitive ELISA is 0.23±0.04 mg·L Pb ion. The cross-reaction with Cd , Cu , Fe , Mn , Zn , and other divalent ions were less than 5%.

关键词： p-SCN-Bz-DTPA     p-NH2-Bn-DTPA     lead ion     polyclonal antibody    

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Development of an H reduction and moderate oxidation method for 3,5-dimethylpyridine hydrogenation in

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1807-1817 doi: 10.1007/s11705-022-2243-2

摘要： The Ru/C catalyst prepared by impregnation method was used for hydrogenation of 3,5-dimethylpyridine in a trickle bed reactor. Under the same reduction conditions (300 °C in H2), the catalytic activity of the non-in-situ reduced Ru/C-n catalyst was higher than that of the in-situ reduced Ru/C-y catalyst. Therefore, an in-situ H2 reduction and moderate oxidation method was developed to increase the catalyst activity. Moreover, the influence of oxidation temperature on the developed method was investigated. The catalysts were characterized by Brunauer–Emmett–Teller method, hydrogen temperature programmed reduction H2-TPR, hydrogen temperature-programmed dispersion (H2-TPD), X-ray diffraction, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, O2 chemisorption and oxygen temperature-programmed dispersion (O2-TPD) analyses. The results showed that there existed an optimal Ru/RuOx ratio for the catalyst, and the highest 3,5-dimethylpyridine conversion was obtained for the Ru/C-i1 catalyst prepared by in-situ H2 reduction and moderate oxidation (oxidized at 100 °C). Excessive oxidation (200 °C) resulted in a significant decrease in the Ru/RuOx ratio of the in-situ H2 reduction and moderate oxidized Ru/C-i2 catalyst, the interaction between RuOx species and the support changed, and the hard-to-reduce RuOx species was formed, leading to a significant decrease in catalyst activity. The developed in-situ H2 reduction and moderate oxidation method eliminated the step of the non-in-situ reduction of catalyst outside the trickle bed reactor.

关键词： Ru/C catalyst     in-situ H2 reduction and moderate oxidation     in-situ reduction     non-in-situ reduction     hydrogenation of 3     5-dimethylpyridine    

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encapsulating M(Co, Fe)-Ni alloy for electrochemical production of syngas with potential-independent CO/H

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 498-510 doi: 10.1007/s11705-021-2082-6

摘要： The electrochemical conversion of CO2-H2O into CO-H2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H2 ratio are highly desired. Herein, a series of N-doped carbon nanotubes encapsulating binary alloy nanoparticles (MxNi-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of melamine and metal precursors. The MxNi-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H2 ratios, from 0.5:1 to 3.4:1, can be produced on MxNi-NCNT. More importantly, stable CO/H2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co1Ni-NCNT and Co2Ni-NCNT, respectively, over a potential window of –0.8 to –1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H2 ratio from electrochemical CO2 reduction.

关键词： electrochemical reduction of CO2     syngas     N-doped carbon nanotubes     encapsulated alloy nanoparticles     CO/H2 ratio    

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

《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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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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标题 作者 时间 类型 操作

Graphene-like -BN supported polyhedral NiS/NiS nanocrystals with excellent photocatalytic 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

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

期刊论文

<i>Ni>-Positive ion activated rapid addition and mitochondrial targeting ratiometric fluorescent probesfor <i>in vivoi> cell H<sub>2sub>S imaging

Yan Shi, Fangjun Huo, Yongkang Yue, Caixia Yin

期刊论文

High specificity detection of Pb

Ruozhen YU,Zheng FANG,Wei MENG,Zhenguang YAN,Lina DU,Hong WANG,Zhengtao LIU

期刊论文

Development of an H reduction and moderate oxidation method for 3,5-dimethylpyridine hydrogenation in

期刊论文

encapsulating M(Co, Fe)-Ni alloy for electrochemical production of syngas with potential-independent CO/H

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

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

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

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

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

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

期刊论文

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

期刊论文