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Improving the ammonia synthesis activity of Ru/CeO_(2) through enhancement of the metal–support interaction

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Journal of Energy Chemistry 2021年第9期30卷 403-409页

作者： Chunyan Li Yuying Shi Zecheng Zhang Jun Ni xiuyun Wang Jianxin Lin Bingyu Lin Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350002FujianChina

The metal–support interactions induced by high-temperature hydrogen reduction have a strong influence on the catalytic performance of ceria-supported Ru catalysts. However, the appearance of the strong metal–support interaction leads to covering of the Ru species by Ce suboxides, which is detrimental to the ammonia synthesis reaction that requires metallic species as active sites. In the present work, the interaction between Ru and ceria in the Ru/CeO_(2) catalyst was induced by NaBH_(4) treatment. NaBH_(4) treatment enhanced the fraction of metallic Ru, proportion of Ce^(3+), content of exposed Ru species, and amount of surface oxygen species. As a result, a larger amount of hydrogen species would desorb by the H_(2)-formation pathway and the strength of hydrogen adsorption would be weaker, weakening the inhibition effect of the hydrogen species on ammonia synthesis. In addition, the strong electronic metal–support interaction aids in nitrogen dissociation. Consequently, Ru/CeO_(2) with NaBH_(4) treatment showed higher ammonia synthesis rates than that with only hydrogen reduction.

关键词： Ammonia synthesis Na BH4treatment Metal–support interaction Ru/CeO_(2)

Triggering in-plane defect cluster on MoS_(2) for accelerated dinitrogen electroreduction to ammonia

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Journal of Energy Chemistry 2021年第11期30卷 359-366,I0008页

作者： Wanru Liao Ke Xie Lijuan Liu xiuyun Wang Yu Luo Shijing Liang Fujian Liu Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002FujianChina Qingyuan Innovation Laboratory Quanzhou 362801FujianChina College of Chemistry Fuzhou UniversityFuzhou 350108FujianChina

Electrochemical nitrogen reduction reaction (eNRR) is an alternative promising manner for sustainable N2 fixation with low-emission. The major challenge for developing an efficient electrocatalyst is the cleaving of the stable Ntriple bondN triple bonds. Herein, we design a new MoS_(2) with in-plane defect cluster through a bottom-up approach for the first time, where the defect cluster is composed of three adjacent S vacancies. The well-defined in-plane defect clusters could contribute to the strong chemical adsorption and activation towards inert nitrogen, achieving an excellent eNRR performance with an ammonia yield rate of 43.4 ± 3 μg h^(−1) mgcat.^(−1) and a Faradaic efficiency of 16.8 ± 2% at −0.3 V (vs. RHE). The performance is much higher than that of MoS_(2) with the edge defect. Isotopic labeling confirms that N atoms of produced NH4+ originate from N2. Furthermore, the in-plane defect clusters realized the alternate hydrogenation of nitrogen in a side-on way to synthesize ammonia. This work provides a prospecting strategy for fine-tuning in-plane defects in a catalyst, and also promotes the progress of eNRR.

关键词： In-plane defect clusters Ammonia synthesis MoS_(2) Electrocatalysis Isotopic labeling

Effect of pore-size distribution on Ru/ZSM-5 catalyst for enhanced N2 activation to ammonia via dissociative mechanism

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Journal of Rare Earths 2020年第8期38卷 873-882,I0002页

作者： Jihui Cai Congying Wang Yi Liu Jun Ni Bingyu Lin xiuyun Wang Jianxin Lin Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002China

In the present study,a series of Ru/ZSM-5 catalysts with different pore-size distributions were prepared and investigated for NH3 *** studies indicate that Ru/ZSM-5-Mic with micropore structure exhibits superior NH3 synthesis rate,which is much higher than those of Ru/ZSM-5-Mac(with macroporous structure)and Ru/ZSM-5-Mes(with mesoporous structure)catalysts.A series of TPD experiments demonstrate that pore-size distributions play an important role in N2 adsorption and activation over Ru/***,the addition of La significantly promotes the NH3 synthesis performance over Ru/***,in situ DRIFTS studies indicate that the main intermediate species over Ru/ZSM-5-Mic are-NH2,and most of the surface hydrogen species desorb following the H2O-formation pathway.

关键词： Ru/ZSM-5 La Ammonia synthesis Pore-size distribution Reaction pathway Rare earths

牛分枝杆菌cfp10-esat6-cfp7融合基因的原核表达及抗原反应性分析

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黑龙江畜牧兽医 2020年第22期 71-76页

作者：张健宁方诗文刘思怡包艳红姚宇黄永顺王春芳姜秀云马红霞吉林农业大学生命科学学院长春130118 吉林农业大学动物科技学院长春130118 长春科技学院长春130600 吉林省新兽药研发与创制重点实验室长春130118

为了增强单个蛋白在牛结核病诊断中的敏感性和抗感染中的免疫原性,试验采用重叠延伸PCR将牛分枝杆菌cfp10基因与esat6基因融合,得到cfp10-esat6融合基因,再行重叠延伸PCR将cfp10-esat6融合基因与cfp7基因融合,得到融合基因cfp10-esat6-c... 详细信息

为了增强单个蛋白在牛结核病诊断中的敏感性和抗感染中的免疫原性,试验采用重叠延伸PCR将牛分枝杆菌cfp10基因与esat6基因融合,得到cfp10-esat6融合基因,再行重叠延伸PCR将cfp10-esat6融合基因与cfp7基因融合,得到融合基因cfp10-esat6-cfp7,并克隆至T-Vector pMD19中,构建重组质粒pMD-cfp10-esat6-cfp7。对pMD-cfp10-esat6-cfp7和pET-28a(+)进行BamHⅠ和EcoRⅠ双酶切,将纯化的cfp10-esat6-cfp7连接到pET-28a(+)中,获得表达质粒pET-cfp10-esat6-cfp7,通过IPTG诱导,SDS-PAGE分析表达质粒在*** BL21(DE3)中的表达情况。对表达的融合蛋白进行镍柱纯化,通过Western-blot和间接ELISA分析其抗原反应性。结果表明:获得了融合基因cfp10-esat6-cfp7,表达了约36.3 ku的融合蛋白CFP10-ESAT6-CFP7。融合蛋白CFP10-ESAT6-CFP7与10份牛结核阳性血清反应的OD492值均在0.6以上,而融合蛋白CFP10-ESAT6与阳性血清反应的OD492值在0.1~0.3之间;融合蛋白CFP10-ESAT6-CFP7与10份牛结核阴性血清的OD492值也明显高于CFP10-ESAT6,其与牛结核阳性血清呈现良好的反应性。说明CFP10-ESAT6-CFP7融合蛋白具有作为牛结核病诊断抗原用于新型疫苗研究的潜在价值。

关键词：牛分枝杆菌 cfp10基因 esat6基因 cfp7基因融合基因原核表达

Highly efficient subnanometer Ru-based catalyst for ammonia synthesis via an associative mechanism

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Chinese Journal of Chemical Engineering 2022年第3期35卷 177-184页

作者： Yanliang Zhou Qianjin Sai Zhenni Tan Congying Wang xiuyun Wang Bingyu Lin Jun Ni Jianxin Lin Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002China

The industrial manufacture of ammonia(NH_(3))using Fe-based catalyst works under rigorous *** the goal of carbon-neutrality,it is highly desired to develop advanced catalyst for NH_(3)synthesis at mild conditions to reduce energy consumption and CO_(2)***,the main challenge of NH_(3)synthesis at mild conditions lies in the dissociation of steady N≡N triple *** this work,we report the design of subnanometer Ru clusters(0.8 nm)anchored on the hollow N-doped carbon spheres catalyst(Ru-SNCs),which effectively promotes the NH_(3)synthesis at mild conditions via an associative *** NH_(3)synthesis rate over Ru-SNCs(0.49%(mass)Ru)reaches up to 11.7 mmol NH_(3)·(g cat)^(-1)·h^(-1) at 400℃ and 3 MPa,which is superior to that of 8.3 mmol NH_(3)·(g cat)^(-1)·h^(-1) over Ru nanoparticle catalyst(1.20%(mass)Ru).Various characterizations show that the N_(2)H_(4)species are the main intermediates for NH_(3)synthesis on Ru-SNCs *** demonstrates that Ru-SNCs catalyst can follow an associative route for N_(2)activation,which circumvents the direct dissociation of N_(2)and results in highly efficient NH_(3)synthesis at mild conditions.

关键词： Ammonia synthesis Sustainability Subnanometer Ru clusters Associative route Catalysis

Hydrogen production from ammonia decomposition over Ni/CeO_(2) catalyst:Effect of CeO_(2) morphology

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Journal of Rare Earths 2023年第7期41卷 1014-1021,I0002页

作者： Chongqi Chen Xiaoshuang Fan Chen Zhou Li Lin Yu Luo Chaktong Au Guohui Cai xiuyun Wang Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002China

Ammonia(NH_(3)) decomposition to release CO_x-free hydrogen(H_(2)) over non-noble catalysts has gained increasing *** this study,three nanostructured CeO_(2) with different morphologies,***(R).sphere(Sph),and spindle(Spi),were fabricated and served as supports for Ni/CeO_(2) *** CeO_(2)supports are different in particle sizes,specific surface area and porosity,resulting in the formation of Ni nanoparticles with distinguished sizes and *** surface properties of the Ni/CeO_(2) catalysts are not only distinct but also influential,affecting the adsorption and desorption of NH_(3),N_(2),and/or H_(2)*** Ni/CeO_(2)-R catalyst shows superior catalytic activity compared to the other two,owing to its smaller Ni crystallite size and larger BET surface *** most abundant strong basic sites are observed for Ni/CeO_(2)-Spi catalyst based on its exposed CeO_(2)(110) planes,which facilitates the donation of electrons to the Ni particles,benefiting the associative desorption of N ***,Ni/CeO_(2)-Spi shows higher catalytic activity than Ni/CeO_(2)-Sph,despite their almost identical Ni crystallite sizes.

关键词： NH_(3)decomposition Hydrogen production Ni/CeO_(2) Morphology Electron donation Rare earths

Target-oriented confinement of Ru-Co nanoparticles inside N-doped carbon spheres via a benzoic acid guided process for high-efficient low-temperature ammonia synthesis

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Journal of Energy Chemistry 2021年第6期30卷 140-146,I0005页

作者： Jun Ni Zhenni Tan Qianjin Sai Jie Zhu xiuyun Wang Bingyu Lin Jianxin Lin Chak-tong Au Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002FujianChina

Ru-based heterogeneous catalysts have been used in a wide range of important ***,due to the sintering of Ru nanoparticles their practical applications are somewhat ***,for the first time we report a new and facile strategy to confine Ru and/or Co nanoparticles(NPs) in the channels of N-doped carbon using benzoic acid to guide the deposition location of *** developed catalyst with confined RuCo alloy particles exhibits high resistance against Ru sintering and displays excellent activity and long term stability for NH3 synthesis,achieving an NH3 synthesis rate of up to 18.9 mmol NH_(3) gcat^(-1)h^(-1)at 400℃,which is ca.2.25 times that of the catalyst prepared without confinement(with metal deposited on the support surface).In the latter case,there is an increase of nanoparticle size from 2.52 to 4.25 nm together with ca.48% decrease of NH_(3) synthesis rate after 68 h at 400℃.This study provides a new avenue for simple fabrication of precious-metal-based catalysts that are highly resistant against sintering,specifically suitable for low-temperature synthesis of ammonia with outstanding efficiency.

关键词： Ru-and Co-based catalysts Ammonia synthesis Confinement Sintering resistance Nanoparticle size

Effects of cerium and tungsten addition on acid-base properties of spindle-likeα-Fe_(2)O_(3)in low-temperature SCR of NO_(x)with NH_(3)

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Journal of Rare Earths 2022年第11期40卷 1734-1742,I0003页

作者： Jun Ni Xuanbei Peng Linlin Yang Kai Zhang Yangyu Zhang Yanliang Zhou xiuyun Wang Chak-tong Au Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhou 350002China

Low-temperature selective catalytic reduction(SCR)is important for the elimination of NOfrom stationary *** the present study,the loading of Ce and W onα-Fe_(2)O_(3)was achieved through the integration of single-mode microwave and incipient wetness impregnation(IWI)*** scanning electron microscopy(SEM)and transmission electron microscopy(TEM)images reveal that the structure ofα-Fe_(2)O_(3)is spindle-like,and the structure remains unchanged after the introduction of Ce and/or *** results of NH-SCR investigation demonstrate that NOconversion over Ce-W/α-Fe_(2)O_(3)is more than85%at 300℃,which is much higher than that over Ce/a-Fe_(2)O_(3)andα-Fe_(2)O_(3),Our studies illustrate that the addition of Ce can significantly increase the amount of surface oxygen vacancies as well as sites of moderate *** the other hand,the addition of W can obviously decrease the amount of basic sites and increase the number of Br?nsted acid *** synergistic effect of Ce and W addition on balancing acidity/basicity properties accounts for the high activity of CeW/α-Fe_(2)O_(3)for NOremoval at low *** study provides insight into the relationship between acidity/basicity properties and catalytic performance of Ce-W/α-Fe_(2)O_(3)catalysts,which is beneficial to the design of high-performance NH-SCR catalyst for NOremoval at low temperatures.

关键词： NH_(3)-SCR Fe_(2)O_(3) NO_(x)removal Acidity/basicity properties Morphology structure Rare earths

Zirconia prepared from UIO-66 as a support of Ru catalyst for ammonia synthesis

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Chinese Chemical Letters 2023年第1期34卷 461-464页

作者： Chuanfeng Zhang Siyu Shi Biyun Fang Jun Ni Jianxin Lin xiuyun Wang Bingyu Lin Lilong jiang National Engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350002China

The development of effective Ru catalyst for ammonia synthesis is of important practical value and scientific significance because of the wide application of ammonia as a fertilizer and its promising applications in the renewable ***,ZrO_(2) was regarded as an inferior support for Ru catalyst used in ammonia *** we prepare ZrO_(2) with monoclinic phase and carbon species from ZrCl_(4) following the preparation route of UiO-66 as well as ammonia *** to the presence of a larger amount of hydrogen adsorption as well as the easier desorption of hydrogen species,the ill effect of hydrogen species on the nitrogen adsorption-desorption and ammonia synthesis can be effectively *** resulting ZrO_(2)-supported Ru catalyst showed 4 times higher ammonia synthesis activity than the conventional Ru/ZrO_(2) obtained from zirconium nitrate.

关键词： Ru catalyst ZrO_(2) Carbon Hydrogen adsorption-desorption Ammonia synthesis