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The modification of titanium in mesoporous silica for Co-based Fischer–Tropsch catalysts

《化学科学与工程前沿（英文）》 2022年 第16卷 第8期   页码 1224-1236 doi: 10.1007/s11705-022-2139-1

摘要： Ordered SBA-15 mesoporous silica with incorporated titanium was successfully synthesized via a one-pot hydrothermal crystallization method. The characterization including powder X-ray diffraction, Brunauer–Emmett–Teller, transmission electron microscope, temperature-programmed reduction, temperature-programmed desorption, Fourier transform infrared and ultraviolet-visible-near infrared spectrometer was performed to explore the physical and chemical structures of both the supports and the catalysts. The results showed that titanium was successfully incorporated into the mesoporous silica framework with a limited amount of titanium (Si/Ti > 20), and the mesoporous structure was retained. However, the increased titanium content inevitably resulted in the formation of anatase TiO 2 particles on the support surface. The increased incorporated titanium strengthened the interactions between cobalt species and supports, which was favorable for the cobalt species dispersion, despite the limited cobalt oxide reducibility. The enhanced metal-support interactions were beneficial for the CO/H2 ratio at the active cobalt sites, which facilitated the formation of more C5+ hydrocarbons. This study provides a promising method for support modification with incorporated-heteroatoms for the rational development of Fischer–Tropsch catalysts.

关键词： Fischer–Tropsch synthesis     titanium incorporation     mesoporous silica     metal-support interactions     C5+ selectivity    

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Enhancing the aromatic selectivity of cyclohexane aromatization by CO2 coupling

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1801-1808 doi: 10.1007/s11705-023-2325-9

摘要： Improving the aromatic selectivity in the alkane aromatization process is of great importance for its practical utilization but challenge to make because the high H/C ratio of alkanes would lead to a serious hydrogen transfer process and a large amount of light alkanes. Herein, CO2 is introduced into the cyclohexane conversion process on the HZSM-5 zeolite, which can improve the aromatic selectivity. By optimizing the reaction conditions, an improved aromatic (benzene, toluene, xylene, and C9+) selectivity of 48.2% can be obtained at the conditions of 2.7 MPa (CO2), 450 °C, and 1.7 h−1, which is better than that without CO2 (aromatic selectivity = 43.2%). In situ transmission Fourier transform infrared spectroscopy spectra illustrate that many oxygenated chemical intermediates (e.g., carboxylic acid, anhydride, unsaturated aldehydes/ketones or ketene) would be formed during the cyclohexane conversion process in the presence of CO2. 13C isotope labeling experimental results demonstrate that CO2 can enter into the aromatics through the formation of oxygenated chemical intermediates and thereby improve the aromatic selectivity. This study may open a green, economic, and promising way to improve the aromatic selectivity for alkane aromatization process.

关键词： aromatics     carbon dioxide     aromatization     coupling reaction     ZSM-5 zeolite    

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Adsorption selectivity of salicylic acid and 5-sulfosalicylic acid onto hypercrosslinked polymeric adsorbents

LIU Fuqiang, CHEN Jinlong, LI Aimin, XIA Mingfang, FEI Zhenghao

《环境科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 73-78 doi: 10.1007/s11783-007-0014-4

摘要： Both bottle-point and column-feeding experiments involving different solutes and sorbents were carried out to investigate the adsorption selectivity and separation performance of salicylic acid and 5-sulfosalicylic acid. Their adsorption isotherms onto such hypercrosslinked polymeric adsorbents as NDA-100 and NDA-99 could be well described by the Freundlich equations whose characteristics describe extrathermic and favorable adsorption processes. The adsorption towards NDA-100 mainly depended on the π-π interaction, while that towards NDA-99 was extremely influenced by the static-electric interaction. Additionally, the adsorptive capacity of salicylic acid on NDA-99 decreased while it increased on NDA-100 with the presence of 5-sulfosalicylic acid in the adsorptive environment as the competitive component. Comparatively, the adsorption capacity of 5-sulfosalicylic acid decreased on both resins with salicylic acid as the competitive component. In fact, the difference in the interaction between adsorbent and adsorbate resulted in the straight antagonism on the effective adsorption sites on the adsorbent. In conclusion, the adsorption selectivity of salicylic acid onto NDA-100 was obviously larger than that onto NDA-99 with the existence of 5-sulfosalicylic acid in the adsorptive environment. A satisfactory separation and recovery of tested solutes in aqueous phase could be foreseeably achieved by the sequencing adsorption technique involving NDA-100 as well as NDA-99.

关键词： 5-sulfosalicylic     bottle-point     hypercrosslinked polymeric     satisfactory separation     NDA-100    

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The effect of doping and steam treatment on the catalytic activities of nano-scale H-ZSM-5 in the methanol

Baodong Song, Yongqiang Li, Gang Cao, Zhenhai Sun, Xu Han

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 564-574 doi: 10.1007/s11705-017-1654-y

摘要： In the transformation of methanol to gasoline (MTG), the selectivity to gasoline and the aromatic content in the produced gasoline are important factors. The catalytic activities of steam-treated and non-steam-treated nano-scale H-ZSM-5 (NHZ5) catalysts impregnated with Ag(I), Zn(II) or P(V) have been investigated in a continuous flow fixed bed reactor. The NH -TPD results showed that after impregnation, the Ag/NHZ5, Zn/NHZ5 and P/NHZ5 catalysts contained comparatively more strong, medium-strong and weak acid sites, respectively. Treatment with steam decreased the number of acid sites in all the catalysts, but the pore volumes in the catalysts were larger which improved carbon deposition resistance resulting in prolonged lifetimes. After 6 h of MTG reaction, the selectivity to gasoline for the steam-treated catalysts, , and were 70.5, 68.4 and 68.7 wt-%, respectively, whereas their respective aromatic contents in the produced gasoline were 61.9, 55.4 and 39.0 wt-%. Thus is the most promising catalyst for MTG applications which can meet the China IV gasoline standard that the amount of aromatics in gasoline should be less than 48 wt-%.

关键词： MTG     nano-scale H-ZSM-5     steam treatment     gasoline     selectivity to gasoline    

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RGS16 regulated by let-7c-5p promotes glioma progression by activating PI3K-AKT pathway

《医学前沿（英文）》 2023年 第17卷 第1期   页码 143-155 doi: 10.1007/s11684-022-0929-y

摘要： Gliomas are the most common central nervous system tumours; they are highly aggressive and have a poor prognosis. RGS16 belongs to the regulator of G-protein signalling (RGS) protein family, which plays an important role in promoting various cancers, such as breast cancer, pancreatic cancer, and colorectal cancer. Moreover, previous studies confirmed that let-7c-5p, a well-known microRNA, can act as a tumour suppressor to regulate the progression of various tumours by inhibiting the expression of its target genes. However, whether RGS16 can promote the progression of glioma and whether it is regulated by miR let-7c-5p are still unknown. Here, we confirmed that RGS16 is upregulated in glioma tissues and that high expression of RGS16 is associated with poor survival. Ectopic deletion of RGS16 significantly suppressed glioma cell proliferation and migration both in vitro and in vivo. Moreover, RGS16 was validated as a direct target gene of miR let-7c-5p. The overexpression of miR let-7c-5p obviously downregulated the expression of RGS16, and knocking down miR let-7c-5p had the opposite effect. Thus, we suggest that the suppression of RGS16 by miR let-7c-5p can promote glioma progression and may serve as a potential prognostic biomarker and therapeutic target in glioma.

关键词： RGS16     let-7c-5p     glioma     proliferation     migration    

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Novel mutation c.1210-3C>G in with a poly-T tract of 5T affects mRNA splicing in a Chinese patient

《医学前沿（英文）》 2022年 第16卷 第1期   页码 150-155 doi: 10.1007/s11684-021-0846-5

摘要： Cystic fibrosis (CF) is a rare autosomal recessive disease with only one pathogenic gene cystic fibrosis transmembrane conductance regulator (CFTR). To identify the potential pathogenic mutations in a Chinese patient with CF, we conducted Sanger sequencing on the genomic DNA of the patient and his parents and detected all 27 coding exons of CFTR and their flanking intronic regions. The patient is a compound heterozygote of c.2909G>A, p.Gly970Asp in exon 18 and c.1210-3C>G in cis with a poly-T of 5T (T5) sequence, 3 bp upstream in intron 9. The splicing effect of c.1210-3C>G was verified via minigene assay in vitro, indicating that wild-type plasmid containing c.1210-3C together with T7 sequence produced a normal transcript and partial exon 10-skipping-transcript, whereas mutant plasmid containing c.1210-3G in cis with T5 sequence caused almost all mRNA to skip exon 10. Overall, c.1210-3C>G, the newly identified pathogenic mutation in our patient, in combination with T5 sequence in cis, affects the CFTR gene splicing and produces nearly no normal transcript in vitro. Moreover, this patient carries a p.Gly970Asp mutation, thus confirming the high-frequency of this mutation in Chinese patients with CF.

关键词： cystic fibrosis     CFTR     splicing mutation     minigene    

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Facile controlled synthesis of hierarchically structured mesoporous Li4Ti5O12/C/rGO composites as high-performance

Cehuang FU, Shuiyun SHEN, Ruofei WU, Xiaohui YAN, Guofeng XIA, Junliang ZHANG

《能源前沿（英文）》 2022年 第16卷 第4期   页码 607-612 doi: 10.1007/s11708-021-0798-0

摘要： In this paper, a facile strategy is proposed to controllably synthesize mesoporous Li4Ti5O12/C nanocomposite embedded in graphene matrix as lithium-ion battery anode via the co-assembly of Li4Ti5O12 (LTO) precursor, GO, and phenolic resin. The obtained composites, which consists of a LTO core, a phenolic-resin-based carbon shell, and a porous frame constructed by rGO, can be denoted as LTO/C/rGO and presents a hierarchical structure. Owing to the advantages of the hierarchical structure, including a high surface area and a high electric conductivity, the mesoporous LTO/C/rGO composite exhibits a greatly improved rate capability as the anode material in contrast to the conventional LTO electrode.

关键词： Li4Ti5O12     phenolic-resin-based carbon     mesoporous composite     graphene    

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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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Tuning the catalytic selectivity in electrochemical CO

Jiafang XIE,Yuxi HUANG,Hanqing YU

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 861-866 doi: 10.1007/s11783-014-0742-1

摘要： Electrochemical conversion of CO to hydrocarbons can relieve both environmental and energy stresses. However, electrocatalysts for this reaction usually suffer from a poor product selectivity and a large overpotential. Here we report that tunable catalytic selectivity for hydrocarbon formation could be achieved on Cu nanomaterials with different morphologies. By tuning the electrochemical parameters, either Cu oxide nanowires or nanoneedles were fabricated and then electrochemically reduced to the corresponding Cu nanomaterials. The Cu nanowires preferred the formation of C H , while the Cu nanoneedles favored the production of more CH , rather than C H . Our work provides a facile synthetic strategy for preparing Cu-based nanomaterials to achieve selective CO reduction.

关键词： electrochemical CO2 reduction     Cu oxide     nanostructure     selectivity     hydrocarbon formation    

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An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 950-962 doi: 10.1007/s11705-022-2162-2

摘要： A series of Cu–Ce–Zr catalysts with different Ce contents are applied to the hydrogenation of CO2 to CO/CH3OH products. The Cu–Ce–Zr catalyst with 2 wt% Ce loading shows higher CO selectivity (SCO = 0.0%–87.8%) from 200–300 °C, while the Cu–Ce–Zr catalyst with 8 wt% Ce loading presents higher CO2 conversion ( XCO2 = 5.4%–15.6%) and CH3OH selectivity ( SCH3OH = 97.8%–40.6%). The number of hydroxyl groups and solid solution nature play a significant role in changing the reaction pathway. The solid solution enhances the CO2 adsorption ability. At the CO2 adsorption step, a larger number of hydroxyl groups over the Cu–Ce–Zr catalyst with 8 wt% Ce loading leads to the production of H-containing adsorption species. At the CO2 hydrogenation step, a larger number of hydroxyl groups assists in encouraging the further hydrogenation of intermediate species to CH3OH and improving the hydrogenation rate. Hence, the Cu–Ce–Zr catalyst with 8 wt% Ce loading favors CH3OH selectivity and CO2 activation, while CO is preferred on the Cu–Ce–Zr catalyst with 2 wt% Ce loading, a smaller number of hydroxyl groups and a solid solution nature. Additionally, high-pressure in situ diffuse reflectance infrared Fourier transform spectroscopy shows that CO is produced from formate decomposition and that both monodentate formate and bidentate formate are active intermediate species of CO2 hydrogenation to CH3OH.

关键词： CO2 hydrogenation     Cu–Ce–Zr     hydroxyls     CO/CH3OH selectivity    

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Solar fuel from photo-thermal catalytic reactions with spectrum-selectivity: a review

Sanli TANG, Jie SUN, Hui HONG, Qibin LIU

《能源前沿（英文）》 2017年 第11卷 第4期   页码 437-451 doi: 10.1007/s11708-017-0509-z

摘要： Solar fuel is one of the ideal energy sources in the future. The synergy of photo and thermal effects leads to a new approach to higher solar fuel production under relatively mild conditions. This paper reviews different approaches for solar fuel production from spectrum-selective photo-thermal synergetic catalysis. The review begins with the meaning of synergetic effects, and the mechanisms of spectrum-selectivity and photo-thermal catalysis. Then, from a technical perspective, a number of experimental or theoretical works are sorted by the chemical reactions and the sacrificial reagents applied. In addition, these works are summarized and tabulated based on the operating conditions, spectrum-selectivity, materials, and productivity. A discussion is finally presented concerning future development of photo-thermal catalytic reactions with spectrum-selectivity.

关键词： photo-thermal catalysis     spectrum-selectivity     solar fuel     full-spectrum    

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Non-toxic, high selectivity process for the extraction of precious metals from waste printed circuit

《环境科学与工程前沿（英文）》 2023年 第17卷 第10期 doi: 10.1007/s11783-023-1723-z

摘要：

● Au, Ag and Pd were recovered from WPCBs with high efficiencies.

关键词： Thiosulfate     Printed circuit boards     Precious metals     Leaching     Hydrometallurgy    

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Catalysis of semihydrogenation of acetylene to ethylene: current trends, challenges, and outlook

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1031-1059 doi: 10.1007/s11705-021-2113-3

摘要： Ethylene is an important feedstock for various industrial processes, particularly in the polymer industry. Unfortunately, during naphtha cracking to produce ethylene, there are instances of acetylene presence in the product stream, which poisons the Ziegler–Natta polymerization catalysts. Thus, appropriate process modification, optimization, and in particular, catalyst design are essential to ensure the production of highly pure ethylene that is suitable as a feedstock in polymerization reactions. Accordingly, carefully selected process parameters and the application of various catalyst systems have been optimized for this purpose. This review provides a holistic view of the recent reports on the selective hydrogenation of acetylene. Previously published reviews were limited to Pd catalysts. However, effective new metal and non-metal catalysts have been explored for selective acetylene hydrogenation. Updates on this recent progress and more comprehensive computational studies that are now available for the reaction are described herein. In addition to the favored Pd catalysts, other catalyst systems including mono, bimetallic, trimetallic, and ionic catalysts are presented. The specific role(s) that each process parameter plays to achieve high acetylene conversion and ethylene selectivity is discussed. Attempts have been made to elucidate the possible catalyst deactivation mechanisms involved in the reaction. Extensive reports suggest that acetylene adsorption occurs through an active single-site mechanism rather than via dual active sites. An increase in the reaction temperature affords high acetylene conversion and ethylene selectivity to obtain reactant streams free of ethylene. Conflicting findings to this trend have reported the presence of ethylene in the feed stream. This review will serve as a useful resource of condensed information for researchers in the field of acetylene-selective hydrogenation.

关键词： selectivity     hydrogenation     acetylene     ethylene     palladium    

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Transport and selectivity of indium through polymer inclusion membrane in hydrochloric acid medium

Xiaorong Meng, Conghui Wang, Pan Zhou, Xiaoqiang Xin, Lei Wang

《环境科学与工程前沿（英文）》 2017年 第11卷 第6期 doi: 10.1007/s11783-017-0950-6

摘要： In the present paper, a polymer inclusion membrane (PIM) containing polyvinyl chloride (PVC), and bis-(2-ethylhexyl) phosphate (D2EHPA) which was used as extracting agent was used for the recovery of In(III) ions in hydrochloric acid medium. The effects of carrier concentration, feed phase pH, strip phase HCl concentration, temperature on the transport, and the membrane’s stability and thickness were examined. And the conditions for the selective separation of In(III) and Cu(II) were optimized. The results showed that the transport of In(III) across PIM was consistent with the first order kinetics equation, and also it was controlled by both the diffusion of the metal complex in the membrane and the chemical reaction at the interface of the boundary layers. The transport flux ( ) was inversely proportional to the membrane thickness, however, the transport stability improved as the membrane thickness increased. The transport flux of In(III) and Cu(II) was decreased by excessive acidity of feed phase and high concentration of Cl . The selectivity separation coefficient of In(III)/Cu(II) was up to 34.33 when the original concentration of both In(III) and Cu(II) was 80 mg·L as well as the pH of the feed phase and the concentration of Cl in the adjusting context were0.6 and 0.5 mol·L , respectively. Within the range of pH= 1–3, the separation selectivity of In(III)/Cu(II) reached the peak in the case when the Cl concentration was 0.7 mol·L .

关键词： Polymer inclusion membrane     Selective transport     D2EHPA     In(III)     Cu(II)    

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天然气提质过程中可有效回收丙烷和乙烷的高工业应用潜力金属有机框架材料 Article

咸士凯, 彭俊杰, Haardik Pandey, Timo Thonhauser, 王浩, 李静

《工程（英文）》 2023年 第23卷 第4期   页码 56-63 doi: 10.1016/j.eng.2022.07.017

摘要： 我们证明了高表面极性和合适孔径是协同提高分离性能的两个关键因素，例如，金属有机框架（MOF）-303 和MIL-160（MIL：拉瓦锡材料研究所）都具有一维（1D）开放通道，其具有高密度杂原子和所需的孔径（5~值得注意的是，MOF-303 在298 K和5 kPa 下对C3H8的吸收高达3.38 mmol∙g−1，C3H8/CH4 (5:85, V/V)理想吸附溶液理论（IAST）选择性为5114，在所有已报道的MOF中创下新高。C3H8和C2H6的高负载能力和选择性。此外，这两种化合物的合成都可以很容易地通过一锅反应来放大规模，从而获得约5 g 的高结晶度样品。

关键词： 金属-有机框架，烃类吸附和分离，选择性，稳定性，放大合成    

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标题 作者 时间 类型 操作

The modification of titanium in mesoporous silica for Co-based Fischer–Tropsch catalysts

期刊论文

Enhancing the aromatic selectivity of cyclohexane aromatization by CO2 coupling

期刊论文

Adsorption selectivity of salicylic acid and 5-sulfosalicylic acid onto hypercrosslinked polymeric adsorbents

LIU Fuqiang, CHEN Jinlong, LI Aimin, XIA Mingfang, FEI Zhenghao

期刊论文

The effect of doping and steam treatment on the catalytic activities of nano-scale H-ZSM-5 in the methanol

Baodong Song, Yongqiang Li, Gang Cao, Zhenhai Sun, Xu Han

期刊论文

RGS16 regulated by let-7c-5p promotes glioma progression by activating PI3K-AKT pathway

期刊论文

Novel mutation c.1210-3C>G in with a poly-T tract of 5T affects mRNA splicing in a Chinese patient

期刊论文

Facile controlled synthesis of hierarchically structured mesoporous Li4Ti5O12/C/rGO composites as high-performance

Cehuang FU, Shuiyun SHEN, Ruofei WU, Xiaohui YAN, Guofeng XIA, Junliang ZHANG

期刊论文

Effects of ancillary ligands in acceptorless benzyl alcohol dehydrogenation mediated by phosphine-free cobalt complexes

期刊论文

Tuning the catalytic selectivity in electrochemical CO

Jiafang XIE,Yuxi HUANG,Hanqing YU

期刊论文

An investigation of the CHOH and CO selectivity of CO hydrogenation over Cu–Ce–Zr catalysts

期刊论文

Solar fuel from photo-thermal catalytic reactions with spectrum-selectivity: a review

Sanli TANG, Jie SUN, Hui HONG, Qibin LIU

期刊论文

Non-toxic, high selectivity process for the extraction of precious metals from waste printed circuit

期刊论文

Catalysis of semihydrogenation of acetylene to ethylene: current trends, challenges, and outlook

期刊论文

Transport and selectivity of indium through polymer inclusion membrane in hydrochloric acid medium

Xiaorong Meng, Conghui Wang, Pan Zhou, Xiaoqiang Xin, Lei Wang

期刊论文

天然气提质过程中可有效回收丙烷和乙烷的高工业应用潜力金属有机框架材料

咸士凯, 彭俊杰, Haardik Pandey, Timo Thonhauser, 王浩, 李静

期刊论文