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Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst for overall water splitting

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1707-1717 doi: 10.1007/s11705-023-2308-x

摘要： Water electrolysis technology is considered to be one of the most promising means to produce hydrogen. Herein, aiming at the problems of high overpotential and slow kinetics in water splitting, N-doped porous carbon nanofibers-coupled CoNi2S4 nanoparticles are prepared as bifunctional electrocatalyst. In the strategy, NaCl is used as the template to prepare porous carbon nanofibers with a large surface area, and sulfur vacancies are created to modulate the electronic structure of CoNi2S4. Electron spin resonance confirms the formation of abundant sulfur vacancies, which largely reduce the bandgap of CoNi2S4 from 1.68 to 0.52 eV. The narrowed bandgap is conducive to the migration of valence electrons and decreases the charge transfer resistance for electrocatalytic reaction. Moreover, the uniform distribution of CoNi2S4 nanoparticles on carbon nanofibers can prevent the aggregation and facilitate the exposure of electrochemical active sites. Therefore, the composite catalyst exhibits low overpotentials of 340 mV@100 mA·cm–2 for oxygen evolution reaction and 380 mV@100 mA·cm–2 for hydrogen evolution reaction. The assembled electrolyzer requires 1.64 V to achieve 10 mA·cm–2 for overall water-splitting with good long-term stability. The excellent performance results from the synergistic effect of porous structures, sulfur deficiency, nitrogen doping, and the well-dispersed active component.

关键词： nanoparticle     sulfur vacancy     porous carbon nanofiber     transition metal sulfides     electrolysis    

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Structural engineering of transition metal-based nanostructured electrocatalysts for efficient water

Yueqing Wang, Jintao Zhang

《化学科学与工程前沿（英文）》 2018年 第12卷 第4期   页码 838-854 doi: 10.1007/s11705-018-1746-3

摘要： Water splitting is a highly promising approach for the generation of sustainable, clean hydrogen energy. Tremendous efforts have been devoted to exploring highly efficient and abundant metal oxide electrocatalysts for oxygen evolution and hydrogen evolution reactions to lower the energy consumption in water splitting. In this review, we summarize the recent advances on the development of metal oxide electrocatalysts with special emphasis on the structural engineering of nanostructures from particle size, composition, crystalline facet, hybrid structure as well as the conductive supports. The special strategies relay on the transformation from the metal organic framework and ion exchange reactions for the preparation of novel metal oxide nanostructures with boosting the catalytic activities are also discussed. The fascinating methods would pave the way for rational design of advanced electrocatalysts for efficient water splitting.

关键词： water splitting     structure engineering     metal organic framework     ion exchange     synergistic effect     hybrid structure     conductive supports    

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Crystalline mesoporous transition metal oxides: hard-templating synthesis and application in environmental

Zhen MA, Bei ZHOU, Yu REN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 341-355 doi: 10.1007/s11783-012-0472-1

摘要： Mesoporous silicas such as MCM-41 and SBA-15 possess high surface areas, ordered nanopores, and excellent thermal stability, and have been often used as catalyst supports. Although mesoporous metal oxides have lower surface areas compared to mesoporous silicas, they generally have more diversified functionalities. Mesoporous metal oxides can be synthesized via a soft-templating or hard-templating approach, and these materials have recently found some applications in environmental catalysis, such as CO oxidation, N O decomposition, and elimination of organic pollutants. In this review, we summarize the synthesis of mesoporous transition metal oxides using mesoporous silicas as hard templates, highlight the application of these materials in environmental catalysis, and furnish some prospects for future development.

关键词： mesoporous materials     silica     metal oxide     hard-templating     environmental catalysis    

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Signal promoting role of a p-type transition metal dichalcogenide used for the detection of ultra-trace

Abdolhamid Hatefi-Mehrjardi, Amirkhosro Beheshti-Marnani, Zarrin Es'haghi

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 823-831 doi: 10.1007/s11705-019-1797-0

摘要： A -type transition metal dichalcogenide (WS ) was synthesized and hybridized with graphene oxide via a simple hydrothermal method. The as-prepared material was used to modify a glassy carbon electrode for the fabrication of a simple, stable, and repeatable methylene blue-labeled “signal-off” aptasensor used for the sensitive determination of very low amounts of sodium diclofenac (DCF). The synthetic material, modification process, and role of WS in the current response enhancement were studied by X-ray diffraction, energy-dispersive X-ray spectroscopy, field emission scanning electron microscopy, high resolution transmission electron microscopy, Hall effect, cyclic voltammetry, differential pulse voltammetry, and electrochemical impedance spectroscopy. Subsequently, a wide linear range of DCF concentration (0.5–300 nmol/L), very low limit of detection (0.23 nmol/L), and good selectivity were obtained using the differential pulse voltammetry method with the assembled aptasensor. Finally, the fabricated aptasensor was successfully developed for physiological real samples with significant recoveries.

关键词： labeled aptasensor     transition metal dichalcogenide     graphene oxide     sodium diclofenac    

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Self-supported transition metal phosphide based electrodes as high-efficient water splitting cathodes

Yan Zhang, Jian Xiao, Qiying Lv, Shuai Wang

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 494-508 doi: 10.1007/s11705-018-1732-9

摘要：

Electrolytic water splitting has been considered as a promising technology to produce highly pure H2 by using electrical power produced from wind, solar energy or other fitful renewable energy resources. Combining novel self-supporting structure and high-performance transition metal phosphides (TMP) shows substantial promise for practical application in water splitting. In this review, we try to provide a comprehensive analysis of the design and fabrication of various self-supported TMP electrodes for hydrogen evolution reaction, which are divided into three categories: catalysts growing on carbon-based substrates, catalysts growing on metal-based substrates and freestanding catalyst films. The material structures together with catalytic performances of self-supported electrodes are presented and discussed. We also show the specific strategies to further improve the catalytic performance by elemental doping or incorporation of nanocarbons. The simple and one-step methods to fabricate self-supported TMP electrodes are also highlighted. Finally, the challenges and perspectives for self-supported TMP electrodes in water splitting application are briefly discussed.

关键词： transition metal phosphide     self-supported electrode     electrocatalysis     hydrogen evolution reaction    

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Promotion of transition metal oxides on the NH

Weiman Li, Haidi Liu, Yunfa Chen

《环境科学与工程前沿（英文）》 2017年 第11卷 第2期 doi: 10.1007/s11783-017-0914-x

摘要： Manganese and chromium oxides promote the NH -SCR activity of Zr-Ce mixed oxide. Cr-Zr-Ce mixed oxide exhibited>80% NO conversion at a wide temperature window. More acid sites and higher reducibility may responsible for the high SCR ability. Chromium oxide and manganese oxide promoted ZrO -CeO catalysts were prepared by a homogeneous precipitation method for the selective catalytic reduction of NO with NH . A series of characterization including X-ray diffraction (XRD), high-resolution transmission electron microscope (HR-TEM), Brunauer–Emmett–Teller (BET) surface area analysis, H temperature-programmed reduction (H -TPR), and X-ray photoelectron spectroscopy (XPS) were used to evaluate the influence of the physicochemical properties on NH -SCR activity. Cr-Zr-Ce and Mn-Zr-Ce catalysts are much more active than ZrO -CeO binary oxide for the low temperature NH -SCR, mainly because of the high specific surface area, more surface oxygen species, improved reducibility derived from synergistic effect among different elements. Mn-Zr-Ce catalyst exhibited high tolerance to SO and H O. Cr-Zr-Ce mixed oxide exhibited>80% NO conversion at a wide temperature window of 100°C–300°C. DRIFT studies showed that the addition of Cr is beneficial to the formation of Bronsted acid sites and prevents the formation of stable nitrate species because of the presence of Cr . The present mixed oxide can be a candidate for the low temperature abatement of NO .

关键词： NH3-selective catalytic reduction     NOx     Low temperature     Cr-Zr-Ce    

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Transition metal-doped heteropoly catalysts for the selective oxidation of methacrolein to methacrylic

Yanxia Zheng,Heng Zhang,Lei Wang,Suojiang Zhang,Shaojun Wang

《化学科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 139-146 doi: 10.1007/s11705-015-1548-9

摘要： Heteropoly compounds with the general formula Cs M H P Mo VO (M= Fe, Co, Ni, Cu or Zn) and Cs Cu H P Mo VO ( = 0.1, 0.3 or 0.7) were synthesized and then used as catalysts for the selective oxidation of methacrolein to methacrylic acid. The effects of the transition metals on the structure and activity of the catalysts were investigated. FTIR spectra showed that the transition metal-doped catalysts maintained the Keggin structure of the undoped catalysts. X-ray diffraction results indicated that before calcination, the catalysts doped with Fe and Cu had cubic secondary structures, while the catalysts doped with Co, Ni or Zn had both triclinic and cubic phases and the Co-doped catalyst had the highest content of the triclinic form. Thermal treatment can decrease the content of the triclinic phase. NH temperature-programmed desorption and H temperature-programmed reduction results showed that the transition metals changed the acid and redox properties of the catalysts. The addition of Fe or Cu had positive effects on the activities of the catalyst which is due to the improvement of the electron transfer between the Fe or Cu and the Mo. The effects of the copper content on structure and catalytic activity were also investigated. The Cs Cu H P Mo VO catalyst had the best performance for the selective oxidation of methacrolein to methacrylic acid.

关键词： heteropoly compounds     transition metals     selective oxidation     methacrolein    

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The capture of carbon dioxide by transition metal aluminates, calcium aluminate, calcium zirconate, calcium

Ganesh TILEKAR, Kiran SHINDE, Kishor KALE, Reshma RASKAR, Abaji GAIKWAD

《化学科学与工程前沿（英文）》 2011年 第5卷 第4期   页码 477-491 doi: 10.1007/s11705-011-1107-y

摘要： The capture of CO by transition metal (Mn, Ni, Co and Zn) aluminates, calcium aluminate, calcium zirconate, calcium silicate and lithium zirconate was carried out at pre- and post-combustion temperatures. The prepared metal adsorbents were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), surface area analysis and acidity/alkalinity measurements. The different experimental variables affecting the adsorbents ability to capture CO , such as the mol ratio of metal ions, the pressure of CO , the exposure time and the temperature of the adsorbent were also investigated. Calcium zirconate captured 13.85 wt-% CO at 650°C and 2.5 atm and calcium silicate captured 14.31 wt-% at 650°C. Molecular sieves (13X) and carbon can only capture a negligible amount of CO at high temperatures (300°C–650°C). However, the mixed metal oxides captured reasonable amount of CO at these higher temperatures. In addition, calcium aluminate, calcium zirconate, calcium silicate and lithium zirconate adsorbents captured CO at both pre and post-combustion temperatures. The trend for the amount of captured carbon dioxide over the adsorbents was calcium aluminate

关键词： captured CO2     pre-combustion temperature     characterization     calcium silicate     calcium zirconate    

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Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NO

Biwu CHU, Jiming HAO, Junhua LI, Hideto TAKEKAWA, Kun WANG, Jingkun JIANG

《环境科学与工程前沿（英文）》 2013年 第7卷 第1期   页码 1-9 doi: 10.1007/s11783-012-0476-x

摘要： Aerosol phase reactions play a very important role on secondary organic aerosol (SOA) formation, and metal-containing aerosols are important components in the atmosphere. In this study, we tested the effects of two transition metal sulfate salts, manganese sulfate (MnSO ) and zinc sulfate (ZnSO ), on the photochemical reactions of a toluene/NO photooxidation system in a 2 m smog chamber. By comparing photochemical reaction products of experiments with and without transition metal sulfate seed aerosols, we evaluated the effects of transition metal sulfate seed aerosols on toluene consumption, NO conversion and the formation of ozone and SOA. MnSO and ZnSO seed aerosols were found to have similar effects on photochemical reactions, both enhance the SOA production, while showing negligible effects on the gas phase compounds. These observations are consistent when varying metal sulfate aerosol concentrations. This is attributed to the catalytic effects of MnSO and ZnSO seed aerosols which may enhance the formation of condensable semivolatile compounds. Their subsequent partitioning into the aerosol phase leads to the observed SOA formation enhancement.

关键词： manganese sulfate     zinc sulfate     seed aerosols     toluene photooxidation     secondary organic aerosol    

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Phosphorus-doped Ni–Co sulfides connected by carbon nanotubes for flexible hybrid supercapacitor

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 491-503 doi: 10.1007/s11705-022-2257-9

摘要： As promising electrode materials for supercapacitors, nickel-cobalt bimetallic sulfides render the advantages of abundant redox reactions and inherently high conductivity. However, in general, unsatisfactory performance of low specific capacity, low rate capability, and fast capacity loss exist in Ni–Co sulfide electrodes. Herein, we rationally regulate phosphorus-doped nickel–cobalt sulfides (P-NCS) to enhance the electrochemical performance by gas–solid phosphorization. Moreover, carbon nanotubes (CNTs) as conductive additives are added to improve the cycle stability and conductivity and form the composite P-NCS/C/CNT. According to density functional theory, more electrons near the Fermi surface of P-NCS are demonstrated notionally than those of simple CoNi2S4. Electrochemical results manifest that P-NCS/C/CNT exhibits superior electrochemical performance, e.g., high specific capacity (932.0 C∙g‒1 at 1 A∙g‒1), remarkable rate capability (capacity retention ratio of 69.1% at 20 A∙g‒1), and lower charge transfer resistance. More importantly, the flexible hybrid asymmetric supercapacitor is assembled using P-NCS/C/CNT and activated carbon, which renders an energy density of 34.875 W·h∙kg‒1 at a power density of 375 W∙kg‒1. These results show that as-prepared P-NCS/C/CNT demonstrates incredible possibility as a battery-type electrode for high-performance supercapacitors.

关键词： cobalt nickel sulfide     phosphorus-doping     hybrid supercapacitor     carbon nanotube     density functional theory    

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Transition metal doped mesoporous titania with a crystalline framework as catalysts for oxidation of

YANG Zehui, OU Encai, WANG Yunan, PENG Li, WANG Jiaqiang, YIN Lihui

《化学科学与工程前沿（英文）》 2008年 第2卷 第3期   页码 296-300 doi: 10.1007/s11705-008-0044-x

摘要： Transition metal M (M = Mn, Fe, Co, Ni, Cu, and Zn) doped mesoporous titania with a crystalline framework was employed as catalysts for the oxidation of -bromotoluene (PBT) to -bromobenzaldehyde (BBD) in acetic acid using aqueous hydrogen peroxide as oxidant. It was found that mesoporous TiO doped with those metals (Fe, Co and Ni) whose atomic radii are relatively smaller exhibited higher conversion rate of PBT. Among these catalysts, the Co/meso-TiO exhibited high substrate conversion and good product (-bromobenzaldehyde) selectivity plus it can be reused once with almost the same activity. The effect of different Ti/Co (molar) ratio on the activities of Co/meso-TiO was also investigated.

关键词： selectivity     conversion     -bromobenzaldehyde     aqueous hydrogen     oxidation    

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In-MOF-derived In2S3/Bi2S3 heterojunction for enhanced photocatalytic hydrogen production

《能源前沿（英文）》 2023年 第17卷 第5期   页码 654-663 doi: 10.1007/s11708-023-0885-5

摘要： Transition metal sulfides are commonly studied as photocatalysts for water splitting in solar-to-fuel conversion. However, the effectiveness of these photocatalysts is limited by the recombination and restricted light absorption capacity of carriers. In this paper, a broad spectrum responsive In2S3/Bi2S3 heterojunction is constructed by in-situ integrating Bi2S3 with the In2S3, derived from an In-MOF precursor, via the high-temperature sulfidation and solvothermal methods. Benefiting from the synergistic effect of wide-spectrum response, effective charge separation and transfer, and strong heterogeneous interfacial contacts, the In2S3/Bi2S3 heterojunction demonstrates a rate of 0.71 mmol/(g∙h), which is 2.2 and 1.7 times as much as those of In2S3 (0.32 mmol/(g∙h) and Bi2S3 (0.41 mmol/(g∙h)), respectively. This paper provides a novel idea for rationally designing innovative heterojunction photocatalysts of transition metal sulfides for photocatalytic hydrogen production.

关键词： photocatalytic hydrogen production     wide-spectrum response     metal sulfides     MOFs derivative     heterogeneous interfacial contact    

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Removal of elemental mercury with Mn/Mo/Ru/Al

Yongfu GUO, Naiqiang YAN, Ping LIU, Shijian YANG, Juan WANG, Zan QU

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 464-473 doi: 10.1007/s11783-012-0430-y

摘要： In this work, a catalytic membrane using Mn/Mo/Ru/Al O as the catalyst was employed to remove elemental mercury (Hg ) from flue gas at low temperature. Compared with traditional catalytic oxidation (TCO) mode, Mn/Al O membrane catalytic system had much higher removal efficiency of Hg . After the incorporation of Mo and Ru, the production of Cl from the Deacon reaction and the retainability for oxidants over Mn/Al O membrane were greatly enhanced. As a result, the oxidization of Hg over Mn/Al O membrane was obviously promoted due to incorporation of Mo and Ru. In the presence of 8 ppmv HCl, the removal efficiency of Hg by Mn/Mo/Ru/Al O membrane reached 95% at 423 K. The influence of NO and SO on Hg removal were insignificant even if 200 ppmv NO and 1000 ppmv SO were used. Moreover, compared with the TCO mode, the Mn/Mo/Ru/Al O membrane catalytic system could remarkably reduce the demanded amount of oxidants for Hg removal. Therefore, the Mn/Mo/Ru/Al O membrane catalytic system may be a promising technology for the control of Hg emission.

关键词： flue gas     elemental mercury     membrane     catalysis     transition metal    

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Epithelial-to-mesenchymal transition in cancer: complexity and opportunities

Yun Zhang, Robert A. Weinberg

《医学前沿（英文）》 2018年 第12卷 第4期   页码 361-373 doi: 10.1007/s11684-018-0656-6

摘要：

The cell-biological program termed the epithelial-to-mesenchymal transition (EMT) plays an important role in both development and cancer progression. Depending on the contextual signals and intracellular gene circuits of a particular cell, this program can drive fully epithelial cells to enter into a series of phenotypic states arrayed along the epithelial-mesenchymal phenotypic axis. These cell states display distinctive cellular characteristics, including stemness, invasiveness, drug-resistance and the ability to form metastases at distant organs, and thereby contribute to cancer metastasis and relapse. Currently we still lack a coherent overview of the molecular and biochemical mechanisms inducing cells to enter various states along the epithelial-mesenchymal phenotypic spectrum. An improved understanding of the dynamic and plastic nature of the EMT program has the potential to yield novel therapies targeting this cellular program that may aid in the management of high-grade malignancies.

关键词： epithelial-to-mesenchymal transition     cancer     metastasis     cancer stem cell    

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Polymerization of methyl methacrylate catalyzed by mono-/bis-salicylaldiminato nickel(II) complexes and methylaluminoxane

Jihong LU, Danfeng ZHANG, Qian CHEN, Buwei YU

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 19-25 doi: 10.1007/s11705-010-0546-1

摘要： Two types of salicylaldiminato-based nickel complexes, mono-ligated Ni(II) complexes ([O-C H - - C(H)=N-Ar]Ni(PPh )(Ph) ( ), [O-(3,5-Br )C H - -C(H)=N-Ar]Ni(PPh )(Ph) ( ), [O-(3- -Bu)C H - -C(H)=N-Ar]Ni(PPh )(Ph) ( )) and bis-ligated Ni(II) complexes ([O-(3,5-Br )C H - -C(H)=N-Ar] Ni ( ), [O-(3,5-Br )C H - -C(H)=N-2-C H (PhO)] Ni ( ), Ar=2,6-C H ( -Pr) ) were synthesized and characterized by Fourier transform infrared spectroscopy (FT-IR), nuclear magnetic resonance (NMR), mass spectrography (MS) and elemental analysis (EA). In the presence of methylaluminoxane (MAO) as cocatalyst, all the nickel complexes exhibited high activities for the polymerization of methyl methacrylate (MMA) and syndiotactic-rich poly(methyl methacrylate) (PMMA) was obtained. The complexes with less bulky substituents on salicylaldiminato framework possessed higher activities, while with the same salicylaldiminato, the mono-ligated nickel complexes showed higher catalytic activity than bis-ligated ones.

关键词： late transition metal catalyst     methyl methacrylate     polymerization     salicylaldiminato nickel complexes     methylaluminoxane     syndiotactic structure    

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标题 作者 时间 类型 操作

Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst for overall water splitting

期刊论文

Structural engineering of transition metal-based nanostructured electrocatalysts for efficient water

Yueqing Wang, Jintao Zhang

期刊论文

Crystalline mesoporous transition metal oxides: hard-templating synthesis and application in environmental

Zhen MA, Bei ZHOU, Yu REN

期刊论文

Signal promoting role of a p-type transition metal dichalcogenide used for the detection of ultra-trace

Abdolhamid Hatefi-Mehrjardi, Amirkhosro Beheshti-Marnani, Zarrin Es'haghi

期刊论文

Self-supported transition metal phosphide based electrodes as high-efficient water splitting cathodes

Yan Zhang, Jian Xiao, Qiying Lv, Shuai Wang

期刊论文

Promotion of transition metal oxides on the NH

Weiman Li, Haidi Liu, Yunfa Chen

期刊论文

Transition metal-doped heteropoly catalysts for the selective oxidation of methacrolein to methacrylic

Yanxia Zheng,Heng Zhang,Lei Wang,Suojiang Zhang,Shaojun Wang

期刊论文

The capture of carbon dioxide by transition metal aluminates, calcium aluminate, calcium zirconate, calcium

Ganesh TILEKAR, Kiran SHINDE, Kishor KALE, Reshma RASKAR, Abaji GAIKWAD

期刊论文

Effects of two transition metal sulfate salts on secondary organic aerosol formation in toluene/NO

Biwu CHU, Jiming HAO, Junhua LI, Hideto TAKEKAWA, Kun WANG, Jingkun JIANG

期刊论文

Phosphorus-doped Ni–Co sulfides connected by carbon nanotubes for flexible hybrid supercapacitor

期刊论文

Transition metal doped mesoporous titania with a crystalline framework as catalysts for oxidation of

YANG Zehui, OU Encai, WANG Yunan, PENG Li, WANG Jiaqiang, YIN Lihui

期刊论文

In-MOF-derived In2S3/Bi2S3 heterojunction for enhanced photocatalytic hydrogen production

期刊论文

Removal of elemental mercury with Mn/Mo/Ru/Al

Yongfu GUO, Naiqiang YAN, Ping LIU, Shijian YANG, Juan WANG, Zan QU

期刊论文

Epithelial-to-mesenchymal transition in cancer: complexity and opportunities

Yun Zhang, Robert A. Weinberg

期刊论文

Polymerization of methyl methacrylate catalyzed by mono-/bis-salicylaldiminato nickel(II) complexes and methylaluminoxane

Jihong LU, Danfeng ZHANG, Qian CHEN, Buwei YU

期刊论文