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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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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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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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A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications

《化学科学与工程前沿（英文）》   页码 1632-1642 doi: 10.1007/s11705-022-2187-6

摘要： Although metal–organic frameworks offer a new platform for developing versatile sorption materials, yet coordinating the functionality, structure and component of these materials remains a great challenge. It depends on a comprehensive knowledge of a “real sorption mechanism”. Herein, a ternary mechanism for U(VI) uptake in metal–organic frameworks was reported. Analogous MIL-100s (Al, Fe, Cr) were prepared and studied for their ability to sequestrate U(VI) from aqueous solutions. As a result, MIL-100(Al) performed the best among the tested materials, and MIL-100(Cr) performed the worst. The nuclear magnetic resonance technique combined with energy-dispersive X-ray spectroscopy and zeta potential measurement reveal that U(VI) uptake in the three metal–organic frameworks involves different mechanisms. Specifically, hydrated uranyl ions form outer-sphere complexes in the surface of MIL-100s (Al, Fe) by exchanging with hydrogen ions of terminal hydroxyl groups (Al-OH2, Fe-OH2), and/or, hydrated uranyl ions are bound directly to Al(III) center in MIL-100(Al) through a strong inner-sphere coordination. For MIL-100(Cr), however, the U(VI) uptake is attributed to electrostatic attraction. Besides, the sorption mechanism is also pH and ionic strength dependent. The present study suggests that changing metal center of metal–organic frameworks and sorption conditions alters sorption mechanism, which helps to construct effective metal–organic frameworks-based sorbents for water purification.

关键词： U(VI)     metal–organic frameworks     adsorption mechanism     metal node    

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Sustainability of metal recovery from E-waste

Biswajit Debnath, Ranjana Chowdhury, Sadhan Kumar Ghosh

《环境科学与工程前沿（英文）》 2018年 第12卷 第6期 doi: 10.1007/s11783-018-1044-9

摘要：

Metal recovery techniques from electronic waste reported in literature.

Metal recovery processes followed in Industries from electronic waste.

Sustainability analysis of metal recovery processes from electronic waste.

关键词： E-waste     Metal recovery     Metal Recovery from E-waste (MREW)     Sustainability    

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Optimizing iodine capture performance by metal–organic framework containing with bipyridine units

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 395-403 doi: 10.1007/s11705-022-2218-3

摘要： Radioactive iodine exhibits medical values in radiology, but its excessive emissions can cause environmental pollution. Thus, the capture of radioiodine poses significant engineering for the environment and medical radiology. The adsorptive capture of radioactive iodine by metal–organic frameworks (MOFs) has risen to prominence. In this work, a Th-based MOF (denoted as Th-BPYDC) was structurally designed and synthesized, consisting of [Th6(μ3-O)4(μ3-OH)4(H2O)6]12+ clusters, abundant bipyridine units, and large cavities that allowed guest molecules diffusion and transmission. Th-BPYDC exhibited the uptake capacities of 2.23 g·g−1 and 312.18 mg·g−1 towards I2 vapor and I2 dissolved in cyclohexane, respectively, surpassing its corresponding analogue Th-UiO-67. The bipyridine units boosted the adsorption performance, and Th-BPYDC showed good reusability with high stability. Our work thus opened a new way for the synthesis of MOFs to capture radioactive iodine.

关键词： metal–organic framework     iodine     adsorption     nuclear waste     environmental remediation    

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Selective capture and separation of xenon and krypton using metal organic frameworks: a review

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1895-1912 doi: 10.1007/s11705-023-2355-3

摘要： Xenon and krypton are widespread useful noble gases in commercial lighting, lasers, electronics, and medical industry. At the same time, radioactive noble gases may proliferate from used nuclear fuel and diffuse in open atmospheres. Metal organic frameworks as hotspot porous materials for gases uptake and separation are considered to be potential solutions. In this review, we comprehensively summarized recent researches on metal organic frameworks for selective capture and separation of xenon and krypton. Particularly, we followed the aspects of different optimal design strategies, including optimal pore/cage size and geometry, open metal sites, ions (anions and cations), and polar functional groups for enhancing the xenon adsorption and separation performances. Meanwhile, a comparison of each strategy and the mechanisms of xenon/krypton separation were pointed out. The separation of krypton from gases mixtures by dual-bed systems was further discussed. Finally, some existing challenges and opportunities for possible real applications were proclaimed.

关键词： metal organic frameworks     xenon     krypton     selective separation     used nuclear fuel    

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Liquid metal thermal hydraulics R&D at European scale: achievements and prospects

《能源前沿（英文）》 2021年 第15卷 第4期   页码 842-853 doi: 10.1007/s11708-021-0743-2

摘要： A significant role for a future nuclear carbon-free energy production is attributed to fast reactors, mostly employing a liquid metal as a coolant. This paper summarizes the efforts that have been undertaken in collaborative projects sponsored by the European Commission in the past 20 years in the fields of liquid-metal heat transfer modeling, fuel assembly and core thermal hydraulics, pool and system thermal hydraulics, and establishment of best practice guidelines and verification, validation, and uncertainty quantification (UQ). The achievements in these fields will be presented along with the prospects on topics which will be studied collaboratively in Europe in the years to come. These prospects include further development of heat transfer models for applied computational fluid dynamics (CFD), further analysis of the consequences of fuel assembly blockages on coolant flow and temperature, analysis of the thermal hydraulic effects in deformed fuel assemblies, extended validation of three-dimensional pool thermal hydraulic CFD models, and further development and validation of multi-scale system thermal hydraulic methods.

关键词： liquid metal     thermal hydraulics     Europe    

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Localized high-concentration electrolytes for lithium metal batteries: progress and prospect

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1354-1371 doi: 10.1007/s11705-022-2286-4

摘要： With the increasing development of digital devices and electric vehicles, high energy-density rechargeable batteries are strongly required. As one of the most promising anode materials with an ultrahigh specific capacity and extremely low electrode potential, lithium metal is greatly considered an ideal candidate for next-generation battery systems. Nevertheless, limited Coulombic efficiency and potential safety risks severely hinder the practical applications of lithium metal batteries due to the inevitable growth of lithium dendrites and poor interface stability. Tremendous efforts have been explored to address these challenges, mainly focusing on the design of novel electrolytes. Here, we provide an overview of the recent developments of localized high-concentration electrolytes in lithium metal batteries. Firstly, the solvation structures and physicochemical properties of localized high-concentration electrolytes are analyzed. Then, the developments of localized high-concentration electrolytes to suppress the formation of dendritic lithium, broaden the voltage window of electrolytes, enhance safety, and render low-temperature operation for robust lithium metal batteries are discussed. Lastly, the remaining challenges and further possible research directions for localized high-concentration electrolytes are outlined, which can promisingly render the practical applications of lithium metal batteries.

关键词： high-concentration electrolyte     localized high-concentration electrolyte     lithium metal battery     solid electrolyte interphase     dendrite    

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Analysis of molten metal spreading and solidification behaviors utilizing moving particle full-implicit

《能源前沿（英文）》 2021年 第15卷 第4期   页码 959-973 doi: 10.1007/s11708-021-0753-0

摘要： To retrieve the fuel debris in Fukushima Daiichi Nuclear Power Plants (1F), it is essential to infer the fuel debris distribution. In particular, the molten metal spreading behavior is one of the vital phenomena in nuclear severe accidents because it determines the initial condition for further accident scenarios such as molten core concrete interaction (MCCI). In this study, the fundamental molten metal spreading experiments were performed with different outlet diameters and sample amounts to investigate the effect of the outlet for spreading-solidification behavior. In the numerical analysis, the moving particle full-implicit method (MPFI), which is one of the particle methods, was applied to simulate the spreading experiments. In the MPFI framework, the melting-solidification model including heat transfer, radiation heat loss, phase change, and solid fraction-dependent viscosity was developed and implemented. In addition, the difference in the spreading and solidification behavior due to the outlet diameters was reproduced in the calculation. The simulation results reveal the detailed solidification procedure during the molten metal spreading. It is found that the viscosity change and the solid fraction change during the spreading are key factors for the free surface condition and solidified materials. Overall, it is suggested that the MPFI method has the potential to simulate the actual nuclear melt-down phenomena in the future.

关键词： molten metal spreading     solidification     particle method     severe accident     fuel debris     decommissioning    

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Visible light responsive photocatalysts developed by substitution with metal cations aiming at artificial

《能源前沿（英文）》 2021年 第15卷 第3期   页码 568-576 doi: 10.1007/s11708-021-0774-8

摘要： To solve resource, energy, and environmental issues, development of sustainable clean energy system is strongly required. In recent years, hydrogen has been paid much attention to as a clean energy. Solar hydrogen production by water splitting using a photocatalyst as artificial photosynthesis is a promising method to solve these issues. Efficient utilization of visible light comprised of solar light is essential for practical use. Three strategies, i.e., doping, control of valence band, and formation of solid solution are often utilized as the useful methods to develop visible light responsive photocatalysts. This mini-review introduces the recent work on visible-light-driven photocatalysts developed by substitution with metal cations of those strategies.

关键词： visible light responsive photocatalyst     water splitting     artificial photosynthesis: metal ion substitution    

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Flow and thermal modeling of liquid metal in expanded microchannel heat sink

《能源前沿（英文）》   页码 796-810 doi: 10.1007/s11708-023-0877-5

摘要： Liquid metal-based microchannel heat sinks (MCHSs) suffer from the low heat capacity of coolant, resulting in an excessive temperature rise of coolant and heat sink when dealing with high-power heat dissipation. In this paper, it was found that expanded space at the top of fins could distribute the heat inside microchannels, reducing the temperature rise of coolant and heat sink. The orthogonal experiments revealed that expanding the top space of channels yielded similar temperature reductions to changing the channel width. The flow and thermal modeling of expanded microchannel heat sink (E-MCHS) were analyzed by both using the 3-dimensional (3D) numerical simulation and the 1-dimensional (1D) thermal resistance model. The fin efficiency of E-MCHS was derived to improve the accuracy of the 1D thermal resistance model. The heat conduction of liquid metal in Z direction and the heat convection between the top surface of fins and the liquid metal could reduce the total thermal resistance (Rt). The above process was effective for microchannels with low channel aspect ratio, low mean velocity (Um) or long heat sink length. The maximum thermal resistance reduction in the example of this paper reached 36.0%. The expanded space endowed the heat sink with lower pressure, which might further reduce the pumping power (P). This rule was feasible both when fins were truncated (h2 < 0, h2 is the height of expanded channel for E-MCHS) and when over plate was raised (h2 > 0).

关键词： liquid metal cooling     heat sink     expanded microchannel     flow and thermal modeling    

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Surface tension of liquid metal: role, mechanism and application

Xi ZHAO, Shuo XU, Jing LIU

《能源前沿（英文）》 2017年 第11卷 第4期   页码 535-567 doi: 10.1007/s11708-017-0463-9

摘要： Surface tension plays a core role in dominating various surface and interface phenomena. For liquid metals with high melting temperature, a profound understanding of the behaviors of surface tension is crucial in industrial processes such as casting, welding, and solidification, etc. Recently, the room temperature liquid metal (RTLM) mainly composed of gallium-based alloys has caused widespread concerns due to its increasingly realized unique virtues. The surface properties of such materials are rather vital in nearly all applications involved from chip cooling, thermal energy harvesting, hydrogen generation, shape changeable soft machines, printed electronics to 3D fabrication, etc. owing to its pretty large surface tension of approximately 700 mN/m. In order to promote the research of surface tension of RTLM, this paper is dedicated to present an overview on the roles and mechanisms of surface tension of liquid metal and summarize the latest progresses on the understanding of the basic knowledge, theories, influencing factors and experimental measurement methods clarified so far. As a practical technique to regulate the surface tension of RTLM, the fundamental principles and applications of electrowetting are also interpreted. Moreover, the unique phenomena of RTLM surface tension issues such as surface tension driven self-actuation, modified wettability on various substrates and the functions of oxides are discussed to give an insight into the acting mechanism of surface tension. Furthermore, future directions worthy of pursuing are pointed out.

关键词： surface tension     liquid metal     soft machine     printed electronics     electrowetting     self-actuation    

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Room temperature liquid metal: its melting point, dominating mechanism and applications

Junheng FU, Chenglin ZHANG, Tianying LIU, Jing LIU

《能源前沿（英文）》 2020年 第14卷 第1期   页码 81-104 doi: 10.1007/s11708-019-0653-8

摘要： The room temperature liquid metal (LM) is recently emerging as a new class of versatile materials with fascinating characteristics mostly originated from its simultaneous metallic and liquid natures. The melting point is a typical parameter to describe the peculiarity of LM, and a pivotal factor to consider concerning its practical applications such as phase change materials (PCMs) and advanced thermal management. Therefore, the theoretical exploration into the melting point of LM is an essential issue, which can be of special value for the design of new LM materials with desired properties. So far, some available strategies such as molecular dynamics (MD) simulation and classical thermodynamic theory have been applied to perform correlative analysis. This paper is primarily dedicated to performing a comprehensive overview regarding typical theoretical strategies on analyzing the melting points. It, then, presents evaluations on several factors like components, pressure, size and supercooling that may be critical for melting processes of liquid metal. After that, it discusses applications associated with the characteristic of low melting points of LM. It is expected that a great many fundamental and practical works are to be conducted in the coming future.

关键词： melting point     liquid metal     crystal     thermodynamics     molecular dynamics    

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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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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

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

期刊论文

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

期刊论文

A ternary mechanism for the facilitated transfer of metal ions onto metal–organic frameworks: implications

期刊论文

Sustainability of metal recovery from E-waste

Biswajit Debnath, Ranjana Chowdhury, Sadhan Kumar Ghosh

期刊论文

Optimizing iodine capture performance by metal–organic framework containing with bipyridine units

期刊论文

Selective capture and separation of xenon and krypton using metal organic frameworks: a review

期刊论文

Liquid metal thermal hydraulics R&D at European scale: achievements and prospects

期刊论文

Localized high-concentration electrolytes for lithium metal batteries: progress and prospect

期刊论文

Analysis of molten metal spreading and solidification behaviors utilizing moving particle full-implicit

期刊论文

Visible light responsive photocatalysts developed by substitution with metal cations aiming at artificial

期刊论文

Flow and thermal modeling of liquid metal in expanded microchannel heat sink

期刊论文

Surface tension of liquid metal: role, mechanism and application

Xi ZHAO, Shuo XU, Jing LIU

期刊论文

Room temperature liquid metal: its melting point, dominating mechanism and applications

Junheng FU, Chenglin ZHANG, Tianying LIU, Jing LIU

期刊论文

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

Yueqing Wang, Jintao Zhang

期刊论文