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Ni particles with phosphorus and adjacent defects catalyze 1,5-dinitronaphthalene hydrogenation with excellentcatalytic performance

Wei Xiong, Susu Zhou, Zeyong Zhao, Fang Hao, Zhihui Cai, Pingle Liu, Hailiang Zhang, Hean Luo

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 998-1007 doi: 10.1007/s11705-020-1994-x

摘要： This work proposes a modified activated carbon support, with defects and heteroatoms (N,P-ACs) by nitrogen and phosphorus doping to load non-noble nickel to catalyze aromatic compound hydrogenation. The Ni/N,P-ACs-900 (prepared at 900 °C) showed promising catalytic activity in liquid-phase 1,5-dinitronaphthalene hydrogenation with a 1,5-diaminonaphthalene yield of 95.8% under the mild condition of 100 °C, which is comparable to the commercial Pd/C catalyst. The nitrogen species were burned off at 900 °C, causing more defects for nickel metal loading, facilitating the interaction between the supports and the nickel metal, and resulting in highly dispersed metal particles. The computational study of the nickel binding energy has been conducted using density functional theory. It exhibits that the defects formed by heteroatom doping are beneficial to nickel anchoring and deposition to form highly uniform nickel particles. The phosphorus species in combination with the defects are suitable for H adsorption and dissociation. These results reveal that the heteroatomic doping on the active carbon shows significant effects in the hydrogenation of the liquid-phase aromatic compounds. These findings could provide a promising route for the rational design of aromatic compound hydrogenation catalysts to significantly decrease the cost by instead using noble metal catalysts in the industry.

关键词： nitrogen and phosphorus doping     non-noble nickel catalyst     aromatic compounds hydrogenation    

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Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

《化学科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 416-420 doi: 10.1007/s11705-007-0076-7

摘要： The favorable microbes for the asymmetric reduction of prochiral aromatic ketones was isolated from soil using acetophenone as the sole carbon source, when the asymmetric reduction of acetophenone (ACP) to chiral ?-phenethyl alcohol (PEA) was chosen as the model reaction. Two microbe strains with excellent catalytic activity were obtained. They were and identified by bacteria identification. The product of the asymmetric reduction of ACP catalyzed by was mainly R-PEA and that by was mainly S-PEA. The yield and enantiomeric excesses (e.e.) could respectively reach 75% and 90% for , and 80% and 70% for , much higher than those catalyzed by baker s yeast.

关键词： excellent catalytic     prochiral aromatic     enantiomeric     -phenethyl     catalytic activity    

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Copolymerization of polyketones catalyzed by polyacrylonitrile resin-supported palladium acetate

GUO Jintang, ZHANG Hongxin, WANG Bo, YE Yaqin

《化学科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 165-170 doi: 10.1007/s11705-008-0010-7

摘要： The crosslinked polyacrylonitrile (PAN) was synthesized by suspension polymerization using acrylonitrile (ANT) and divinylbenzene (DVB). Effects of a variety of conditions on the polymerization of PAN particle size and stiffness were investigated. Polyketone was prepared by the copolymerization of carbon monoxide (CO) and styrene (ST) catalyzed by PAN resin-supported palladium acetate. The resin-supported catalyst and the copolymerization product were characterized by infrared spectroscopy (IR) and Scanning Electron Microscopy (SEM). Effects of the components of a catalytic system and reaction time on the catalytic activity were studied. The reusability of the resin-supported catalyst was also investigated. Results indicated that the resin-supported catalyst has excellent catalytic property. The yield of polyketone was 6.2348 g when using 1 g of resin and 22.4 mg of palladium acetate.

关键词： copolymerization     Electron Microscopy     monoxide     excellent catalytic     Polyketone    

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Efficient acetylene/carbon dioxide separation with excellent dynamic capacity and low regeneration energy

《化学科学与工程前沿（英文）》   页码 1616-1622 doi: 10.1007/s11705-022-2183-x

摘要： Adsorptive separation of acetylene/carbon dioxide mixtures by porous materials is an important and challenging task due to their similar sizes and physical properties. Here, remarkable acetylene/carbon dioxide separation featuring a high dynamic breakthrough capacity for acetylene (4.3 mmol·g–1) as well as an ultralow acetylene regeneration energy (29.5 kJ·mol–1) was achieved with the novel TiF62–-pillared material ZU-100 (TIFSIX-bpy-Ni). Construction of a pore structure with abundant TiF62– anion sites and pores with appropriate sizes enabled formation of acetylene clusters through hydrogen bonds and intermolecular interactions, which afforded a high acetylene capacity (8.3 mmol·g–1) and high acetylene/carbon dioxide uptake ratio (1.9) at 298 K and 1 bar. Moreover, the NbO52– anion-pillared material ZU-61 investigated for separation of acetylene/carbon dioxide. In addition, breakthrough experiments were also conducted to further confirm the excellent dynamic acetylene/carbon dioxide separation performance of ZU-100.

关键词： adsorption     acetylene/carbon dioxide separation     dynamic capacity     anion-pillared hybrid material    

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multifunctional polypyrrole/cellulose nanofiber composite films with outstanding photothermal effect, excellent

《化学科学与工程前沿（英文）》 2023年 第17卷 第8期   页码 1028-1037 doi: 10.1007/s11705-022-2251-2

摘要： Electrodes that combine energy storage with mechanical and photothermal performance are necessary for efficient development and use of flexible energy storage and conversion devices. In this study, the flexible, ultrathin, and multifunctional polypyrrole/cellulose nanofiber composite films were fabricated via a one-step “soak and polymerization” method. The dense sandwich structure and strong interfacial interaction endowed polypyrrole/cellulose nanofiber composite films with excellent flexibility, outstanding mechanical strength, and desired toughness. Interestingly, the polypyrrole/cellulose nanofiber composite film electrodes with quaternary amine functionalized cellulose nanofiber had the highest specific mass capacitance (392.90 F∙g–1) and specific areal capacitance (3.32 F∙cm–2) than the electrodes with unmodified and carboxyl functionalized cellulose nanofibers. Further, the polypyrrole/cellulose nanofiber composite films with sandwich structure had excellent photothermal conversion properties. This study demonstrated a feasible and versatile method for preparing of multifunctional composite films, having promising applications in various energy storage fields.

关键词： cellulose nanofiber     electrochemical     photothermal conversion     polypyrrole    

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Strategic position and development prospects of nuclear energy in China

SHEN Wenquan

《能源前沿（英文）》 2007年 第1卷 第2期   页码 125-128 doi: 10.1007/s11708-007-0015-9

摘要： By analyzing the challenges of China s energy supply, an excellent perspective of nuclear power development in the country has been described. Taking into account the near-, mid-, and long-term development requirements, a comprehensive, coordinated and sustainable nuclear power program is proposed. Thus, our national nuclear industry can not only catch up with the world s advanced level in proper time, but also possess enough stamina for sustainability.

关键词： development     excellent perspective     long-term development     comprehensive     national    

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Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1761-1771 doi: 10.1007/s11705-022-2195-6

摘要： Microbial electrosynthesis is a promising alternative to directly convert CO2 into long-chain compounds by coupling inorganic electrocatalysis with biosynthetic systems. However, problems arose that the conventional electrocatalysts for hydrogen evolution may produce extensive by-products of reactive oxygen species and cause severe metal leaching, both of which induce strong toxicity toward microorganisms. Moreover, poor stability of electrocatalysts cannot be qualified for long-term operation. These problems may result in poor biocompatibility between electrocatalysts and microorganisms. To solve the bottleneck problem, Co anchored on porphyrinic triazine-based frameworks was synthesized as the electrocatalyst for hydrogen evolution and further coupled with Cupriavidus necator H16. It showed high selectivity for a four-electron pathway of oxygen reduction reaction and low production of reactive oxygen species, owing to the synergistic effect of Co–Nx modulating the charge distribution and adsorption energy of intermediates. Additionally, low metal leaching and excellent stability were observed, which may be attributed to low content of Co and the stabilizing effect of metalloporphyrins. Hence, the electrocatalyst exhibited excellent biocompatibility. Finally, the microbial electrosynthesis system equipped with the electrocatalyst successfully converted CO2 to poly-β-hydroxybutyrate. This work drew up a novel strategy for enhancing the biocompatibility of electrocatalysts in microbial electrosynthesis system.

关键词： microbial electrosynthesis     hydrogen evolution reaction     metalloporphyrins     biocompatibility     CO2 conversion    

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Aerobic granulation of pure bacterial strain

ADAV Sunil S., LEE Duu-Jong

《环境科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 461-467 doi: 10.1007/s11783-008-0066-0

摘要： The objective of this study is to cultivate aerobic granules by pure bacterial strain, , in a sequencing batch reactor. Stable granules sized 2.0–2.2 mm were formed in the reactor after a five-week cultivation. These granules exhibited excellent settling attributes, and degraded phenol at rates of 1.49 and 1.19 g phenol/(g VSS·d) at 250 and 1500 mg/L of phenol concentration, respectively. Confocal laser scanning microscopic test results show that was distributed over the initial small aggregates, and the outer edge of the granule was away from the core regime in the following stage.

关键词： following     excellent settling     phenol/     sequencing     microscopic    

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A review on catalytic & non-catalytic bio-oil upgrading in supercritical fluids

Sainab Omar, Yang Yang, Jiawei Wang

《化学科学与工程前沿（英文）》 2021年 第15卷 第1期   页码 4-17 doi: 10.1007/s11705-020-1933-x

摘要： This review article summarizes the key published research on the topic of bio-oil upgrading using catalytic and non-catalytic supercritical fluid (SCF) conditions. The precious metal catalysts Pd, Ru and Pt on various supports are frequently chosen for catalytic bio-oil upgrading in SCFs. This is reportedly due to their favourable catalytic activity during the process including hydrotreating, hydrocracking, and esterification, which leads to improvements in liquid yield, heating value, and pH of the upgraded bio-oil. Due to the costs associated with precious metal catalysts, some researchers have opted for non-precious metal catalysts such as acidic HZSM-5 which can promote esterification in supercritical ethanol. On the other hand, SCFs have been effectively used to upgrade crude bio-oil without a catalyst. Supercritical methanol, ethanol, and water are most commonly used and demonstrate catalyst like activities such as facilitating esterification reactions and reducing solid yield by alcoholysis and hydrolysis, respectively.

关键词： bio-oil     upgrading     supercritical     review    

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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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Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1206-1216 doi: 10.1007/s11705-020-2017-7

摘要： In this work, the detailed oxygen reduction reaction (ORR) catalytic performance of M-N O (M= Fe, Co, and Ni; = 1–4) has been explored via the detailed density functional theory method. The results suggest that the formation energy of M-N O shows a good linear relationship with the number of doped O atoms. The adsorption manner of O on M-N O changed from end-on ( = 1 and 2) to side-on ( = 3 and 4), and the adsorption strength gradually increased. Based on the results for binding strength of ORR intermediates and the Gibbs free energy of ORR steps on the studied catalysts, we screened out two highly active ORR catalysts, namely Co-N O and Ni-N O , which possess very small overpotentials of 0.27 and 0.32 V, respectively. Such activities are higher than the precious Pt catalyst. Electronic structure analysis reveals one of the reasons for the higher activity of Co-N O and Ni-N O is that they have small energy gaps and moderate highest occupied molecular orbital energy levels. Furthermore, the results of the density of states reveal that the O doping can improve the electronic structure of the original catalyst to tune the adsorption of the ORR intermediates.

关键词： M-N-C catalyst     oxygen doping     oxygen reduction reaction     catalytic activity     density functional theory    

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Plasma enhanced chemical vapor deposition of excellent a-Si:H passivation layers for a-Si:H/c-Si heterojunction

Lei ZHAO,Wenbin ZHANG,Jingwei CHEN,Hongwei DIAO,Qi WANG,Wenjing WANG

《能源前沿（英文）》 2017年 第11卷 第1期   页码 85-91 doi: 10.1007/s11708-016-0437-3

摘要： The intrinsic a-Si:H passivation layer inserted between the doped a-Si:H layer and the c-Si substrate is very crucial for improving the performance of the a-Si:H/c-Si heterojunction (SHJ) solar cell. The passivation performance of the a-Si:H layer is strongly dependent on its microstructure. Usually, the compact a-Si:H deposited near the transition from the amorphous phase to the nanocrystalline phase by plasma enhanced chemical vapor deposition (PECVD) can provide excellent passivation. However, at the low deposition pressure and low deposition power, such an a-Si:H layer can be only prepared in a narrow region. The deposition condition must be controlled very carefully. In this paper, intrinsic a-Si:H layers were prepared on n-type Cz c-Si substrates by 27.12 MHz PECVD at a high deposition pressure and high deposition power. The corresponding passivation performance on c-Si was investigated by minority carrier lifetime measurement. It was found that an excellent a-Si:H passivation layer could be obtained in a very wide deposition pressure and power region. Such wide process window would be very beneficial for improving the uniformity and the yield for the solar cell fabrication. The a-Si:H layer microstructure was further investigated by Raman and Fourier transform infrared (FTIR) spectroscopy characterization. The correlation between the microstructure and the passivation performance was revealed. According to the above findings, the a-Si:H passivation performance was optimized more elaborately. Finally, a large-area SHJ solar cell with an efficiency of 22.25% was fabricated on the commercial 156 mm pseudo-square n-type Cz c-Si substrate with the open-circuit voltage ( ) of up to 0.732 V.

关键词： PECVD     high pressure and high power     a-Si:H microstructure     passivation     heterojunction solar cell    

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Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

《环境科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 186-193 doi: 10.1007/s11783-009-0016-5

摘要： The reaction mechanisms of selective catalytic reduction (SCR) of nitric oxide (NO) by methane (CH ) over solid superacid-based catalysts were proposed and testified by DRIFTS studies on transient reaction as well as by kinetic models. Catalysts derived from different supports would lead to different reaction pathways, and the acidity of solid superacid played an important role in determining the reaction mechanisms and the catalytic activities. Higher ratios of Br?nsted acid sites to Lewis acid sites would lead to stronger oxidation of methane and then could facilitate the step of methane activation. Strong Br?nsted acid sites would not necessarily lead to better catalytic performance, however, since the active surface NO species and the corresponding reaction routes were determined by the overall acidity strength of the support. The reaction routes where NO moiety was engaged as an important intermediate involved moderate oxidation of methane, the rate of which could determine the overall activity. The reaction involving NO moiety was likely to be determined by the step of reduction of NO. Therefore, to enhance the SCR activity of solid superacid catalysts, reactions between appropriate couples of active NO species and activated hydrocarbon intermediates should be realized by modification of the support acidity.

关键词： selective catalytic reduction (SCR)     nitric oxide (NO)     methane     support acidity     Br?nsted acid sites     NOy species    

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Preparation of rare-earth metal complex oxide catalysts for catalytic wet air oxidation

LI Ning, LI Guangming, YAO Zhenya, ZHAO Jianfu

《环境科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 190-195 doi: 10.1007/s11783-007-0033-1

摘要： Catalytic wet air oxidation (CWAO) is one of the most promising technologies for pollution abatement. Developing catalysts with high activity and stability is crucial for the application of the CWAO process. The Mn/Ce complex oxide catalysts for CWAO of high concentration phenolcontaining wastewater were prepared by coprecipitation. The catalyst preparation conditions were optimized by using an orthogonal layout method and single-factor experimental analysis. The Mn/Ce serial catalysts were characterized by Brunauer Emmett Teller (BET) analysis and the metal cation leaching was measured by inductively coupled plasma torch-atomic emission spectrometry (ICP-AES). The results show that the catalysts have high catalytic activities even at a low temperature (80?C) and low oxygen partial pressure (0.5 MPa) in a batch reactor. The metallic ion leaching is comparatively low (Mn<6.577 mg/L and Ce<0.6910 mg/L, respectively) in the CWAO process. The phenol, COD, and TOC removal efficiencies in the solution exceed 98.5% using the optimal catalyst (named CSP). The new catalyst would have a promising application in CWAO treatment of high concentration organic wastewater.

关键词： torch-atomic emission     Brunauer     Catalytic     process     stability    

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Properties and catalytic mechanism of -glutamyltranspeptidase from NX-2

WANG Qian, YAO Zhong, XUN Zhijing, XU Xiaoying, XU Hong, WEI Ping

《化学科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 456-461 doi: 10.1007/s11705-008-0075-3

摘要： Since -glutamyltranspeptidase (GGT) especially catalyses the transfer of the -glutamyl moiety to a variety of amino acids and short peptides, GGT has important practical value for enzymatic synthesis of -glutamyl compounds. In this paper, the GGT produced from NX-2 was purified by a combination of ammonium sulfate fractionation and ion exchange chromatography, and the properties of purified GGT were investigated. At the conditions of pH 10.0, D-glutamine (D-Gln)/L-tryptophan (L-Trp) with a molar ratio of 5 : 7, a temperature 40°C and a reaction time of 4 h, a higher conversion rate of 42% was obtained. According to the time course, the catalytic mechanism of enzymatic synthesis of -D-glutamyl-L-tryptophan (-D-Gln-L-Trp) was discussed. It was demonstrated that the GGT can catalyze not only the reaction of transpeptidation, but also the irreversible hydrolysis of the products which results in the decrease of the yield of the products. The affinity parameter of GGT to D-Gln (Km) was 5.08 mmol·L and the maximum reaction rate of transpeptidation () was determined as 0.034 mmol·min·L, while the affinity parameter of GGT to -D-Gln-L-Trp (’) was 2.267 mmol·L, and the maximum reaction rate of hydrolysis (’) was 0.012 mmol·min·L.

关键词： catalytic mechanism     mmol·min·L     D-glutamine     affinity parameter     important practical    

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标题 作者 时间 类型 操作

Ni particles with phosphorus and adjacent defects catalyze 1,5-dinitronaphthalene hydrogenation with excellentcatalytic performance

Wei Xiong, Susu Zhou, Zeyong Zhao, Fang Hao, Zhihui Cai, Pingle Liu, Hailiang Zhang, Hean Luo

期刊论文

Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

期刊论文

Copolymerization of polyketones catalyzed by polyacrylonitrile resin-supported palladium acetate

GUO Jintang, ZHANG Hongxin, WANG Bo, YE Yaqin

期刊论文

Efficient acetylene/carbon dioxide separation with excellent dynamic capacity and low regeneration energy

期刊论文

multifunctional polypyrrole/cellulose nanofiber composite films with outstanding photothermal effect, excellent

期刊论文

Strategic position and development prospects of nuclear energy in China

SHEN Wenquan

期刊论文

Co anchored on porphyrinic triazine-based frameworks with excellent biocompatibility for conversion of

期刊论文

Aerobic granulation of pure bacterial strain

ADAV Sunil S., LEE Duu-Jong

期刊论文

A review on catalytic & non-catalytic bio-oil upgrading in supercritical fluids

Sainab Omar, Yang Yang, Jiawei Wang

期刊论文

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

期刊论文

Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

期刊论文

Plasma enhanced chemical vapor deposition of excellent a-Si:H passivation layers for a-Si:H/c-Si heterojunction

Lei ZHAO,Wenbin ZHANG,Jingwei CHEN,Hongwei DIAO,Qi WANG,Wenjing WANG

期刊论文

Effects of support acidity on the reaction mechanisms of selective catalytic reduction of NO by CH

Shicheng XU, Junhua LI, Dong YANG, Jiming HAO

期刊论文

Preparation of rare-earth metal complex oxide catalysts for catalytic wet air oxidation

LI Ning, LI Guangming, YAO Zhenya, ZHAO Jianfu

期刊论文

Properties and catalytic mechanism of -glutamyltranspeptidase from NX-2

WANG Qian, YAO Zhong, XUN Zhijing, XU Xiaoying, XU Hong, WEI Ping

期刊论文