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Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1196-1207 doi: 10.1007/s11705-022-2289-1

摘要： The electrochemical reduction of NH4HCO3 to syngas can bypass the high energy consumption of high-purity CO2 release and compression after the ammonia-based CO2 capture process. This technology has broad prospects in industrial applications and carbon neutrality. A zeolitic imidazolate framework-8 precursor was introduced with different Ag contents via colloid chemical synthesis. This material was carbonized at 1000 °C to obtain AgZn zeolitic imidazolate framework derived nitrogen carbon catalysts, which were used for the first time for boosting the direct conversion of NH4HCO3 electrolyte to syngas. The AgZn zeolitic imidazolate framework derived nitrogen carbon catalyst with a Ag/Zn ratio of 0.5:1 achieved the highest CO Faradaic efficiency of 52.0% with a current density of 1.15 mA·cm–2 at –0.5 V, a H2/CO ratio of 1–2 (–0.5 to –0.7 V), and a stable catalytic activity of more than 6 h. Its activity is comparable to that of the CO2-saturated NH4HCO3 electrolyte. The highly discrete Ag-Nx and Zn-Nx nodes may have combined catalytic effects in the catalysts synthesized by appropriate Ag doping and sufficient carbonization. These nodes could increase active sites of catalysts, which is conducive to the transport and adsorption of reactant CO2 and the stability of *COOH intermediate, thus can improve the selectivity and catalytic activity of CO.

关键词： Ag catalyst     zeolitic imidazolate framework     CO2 electroreduction     ammonium bicarbonate electrolyte     syngas    

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Zeolitic imidazolate framework-8 (ZIF-8) for drug delivery: A critical review

Simin Feng, Xiaoli Zhang, Dunyun Shi, Zheng Wang

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 221-237 doi: 10.1007/s11705-020-1927-8

摘要： Zeolitic imidazolate framework-8 (ZIF-8), composed of Zn ions and imidazolate ligands, is a class of metal-organic frameworks, which possesses a similar structure as conventional aluminosilicate zeolites. This material exhibits inherent porous property, high loading capacity, and pH-sensitive degradation, as well as exceptional thermal and chemical stability. Extensive research effort has been devoted to relevant research aspects ranging from synthesis methods, property characterization to potential applications of ZIF-8. This review focuses on the recent development of ZIF-8 synthesis methods and its promising applications in drug delivery. The potential risks of using ZIF-8 for drug delivery are also summarized.

关键词： zeolitic imidazolate framework-8 (ZIF-8)     synthesis methods     applications     drug delivery    

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Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient

《化学科学与工程前沿（英文）》 2023年 第18卷 第1期 doi: 10.1007/s11705-023-2378-9

摘要： In this study, we synthesize a catalyst comprising cobalt nanoparticles supported on MXene by pyrolyzing a composite in a N2 environment. Specifically, the composite comprises a bimetallic Zn/Co zeolitic imidazole framework grown in situ on the outer surface of MXene. The catalytic efficiency of the catalyst is tested for the self-coupling of 4-methoxybenzylamine to produce value-added imine, where atmospheric oxygen (1 atm) is used as the oxidant. Based on the results, the catalyst displayed impressive catalytic activity, achieving 95.4% yield of the desired imine at 383 K for 8 h. Furthermore, the catalyst showed recyclability and tolerance toward benzylamine substrates with various functional groups. The outstanding performance of the catalyst is primarily attributed to the synergetic catalytic effect between the cobalt nanoparticles and MXene support, while also benefiting from the three-dimensional porous structure. Additionally, a preliminary investigation of potential reaction mechanisms is conducted.

关键词： MXene     sacrificial template     oxidative self-coupling     Co nanoparticles     imine    

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Parametric study on the mixed solvent synthesis of ZIF-8 nano- and micro-particles for CO adsorption: A response surface study

Alireza Hadi, Javad Karimi-Sabet, Abolfazl Dastbaz

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 579-594 doi: 10.1007/s11705-018-1770-3

摘要： The room temperature synthesis of ZIF-8 micro- and nano-particles was investigated using a mixed methanol-water solvent system. ZIF-8 particles of good quality and high crystallinity were obtained. Response surface methodology was used to determine the effect of the synthesis conditions on the ZIF-8 yield, particle size distribution, and mean particle size. The ligand/metal salt molar ratio followed by the amount of sodium formate (the deprotonating agent) and then the amount of water (i.e., the composition of the mixed solvent) respectively had the largest effects on both the ZIF-8 yield and particle size. Results showed that mixing of solvents with different strengths in producing ZIF-8 crystals is a practical method to size-controlled synthesis of ZIF-8 particles. This method is more favorable for industrial-scale ZIF-8 synthesis than using excess amounts of ligands or chemical additives (like sodium formate). In addition, ZIF-8 samples with different mean particle sizes (100, 500, and 1000 nm) were used for CO adsorption and the mid-sized ZIF-8 particles had the highest adsorption capacity.

关键词： metal organic frameworks     zeolitic imidazolate frameworks     ZIF-8     response surface methodology     Box Behnken design     CO adsorption    

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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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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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Metal-organic frameworks for CO

Lei ZHANG, Junqing ZHANG

《能源前沿（英文）》 2019年 第13卷 第2期   页码 221-250 doi: 10.1007/s11708-019-0629-8

摘要： Metal-organic frameworks (MOFs) have attracted much attention because of their large surface areas, tunable structures, and potential applications in many areas. In recent years, MOFs have shown much promise in CO photoreduction. This review summarized recent research progresses in MOF-based photocatalysts for photocatalytic reduction of CO . Besides, it discussed strategies in rational design of MOF-based photocatalysts (functionalized pristine MOFs, MOF-photosensitizer, MOF- semiconductor, MOF-metal, and MOF-carbon materials composites) with enhanced performance on CO reduction. Moreover, it explored challenges and outlook on using MOF-based photocatalysts for CO reduction.

关键词： metal-organic frameworks (MOFs)     photocatalysis     CO2 photoreduction     composite    

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Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 570-580 doi: 10.1007/s11705-022-2247-y

摘要： Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe2Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe2Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO2(110) catalysts. The analysis of the potential gap of Fe2M clusters indicates that Fe2Mn, Fe2Co, and Fe2Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe2Mn and Fe2Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe2M–PCN–Fe2M is explored. Compared with Fe2Mn–PCN–Fe2Mn, Fe2Co–PCN–Fe2Co, and isolated Fe2M clusters, the mixed-metal Fe2Co–PCN–Fe2Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe2Co–PCN–Fe2Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词： bimetallic metal–organic frameworks     bifunctional electrocatalyst     density functional theory     oxygen reduction reaction     oxygen evolution reaction    

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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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Crystalline porous materials: from zeolites to metal-organic frameworks (MOFs)

Zaiku Xie, Bao-Lian Su

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 123-126 doi: 10.1007/s11705-020-1921-1

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Hierarchical porous metal-organic frameworks/polymer microparticles for enhanced catalytic degradation

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 939-949 doi: 10.1007/s11705-022-2152-4

摘要： This work reports on a simple microfluidic strategy to controllably fabricate uniform polymeric microparticles containing hierarchical porous structures integrated with highly accessible catalytic metal organic frameworks for efficient degradation of organic contaminants. Monodisperse (W1/O)/W2 emulsion droplets generated from microfluidics are used as templates for the microparticle synthesis. The emulsion droplets contain tiny water microdroplets from homogenization and water nanodroplets from diffusion-induced swollen micelles as the dual pore-forming templates, and Fe-based metal-organic framework nanorods as the nanocatalysts. The obtained microparticles possess interconnected hierarchical porous structures decorated with highly accessible Fe-based metal-organic framework nanorods for enhanced degradation of organic contaminants via a heterogeneous Fenton-like reaction. Such a degradation performance is highlighted by using these microparticles for efficient degradation of rhodamine B in hydrogen peroxide solution. This work provides a simple and general strategy to flexibly combine hierarchical porous structures and catalytic metal-organic frameworks to engineer advanced microparticles for water decontamination.

关键词： metal-organic framework     polymer microparticle     nanocatalyst     decontamination     organic contaminant    

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Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1487-1499 doi: 10.1007/s11705-021-2085-3

摘要： Developing cost-effective electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital in energy conversion and storage applications. Herein, we report a simple method for the synthesis of graphene-reinforced CoS/C nanocomposites and the evaluation of their electrocatalytic performance for typical electrocatalytic reactions. Nanocomposites of CoS embedded in N, S co-doped porous carbon and graphene (CoS@C/Graphene) were generated via simultaneous sulfurization and carbonization of one-pot synthesized graphite oxide-ZIF-67 precursors. The obtained CoS@C/Graphene nanocomposites were characterized by X-ray diffraction, Raman spectroscopy, thermogravimetric analysis-mass spectroscopy, scanning electronic microscopy, transmission electronic microscopy, X-ray photoelectron spectroscopy and gas sorption. It is found that CoS nanoparticles homogenously dispersed in the in situ formed N, S co-doped porous carbon/graphene matrix. The CoS@C/10Graphene composite not only shows excellent electrocatalytic activity toward ORR with high onset potential of 0.89 V, four-electron pathway and superior durability of maintaining 98% of current after continuously running for around 5 h, but also exhibits good performance for OER and HER, due to the improved electrical conductivity, increased catalytic active sites and connectivity between the electrocatalytic active CoS and the carbon matrix. This work offers a new approach for the development of novel multifunctional nanocomposites for the next generation of energy conversion and storage applications.

关键词： MOF derivative     graphene     electrocatalyst     oxygen reduction reaction     oxygen evolution reaction     hydrogen evolution reaction    

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Rethinking the tendering frameworks of construction contractors in the context of a soft systems methodology

Stephen URQUHART, Andrew WHYTE

《工程管理前沿（英文）》 2018年 第5卷 第3期   页码 369-380 doi: 10.15302/J-FEM-2018019

摘要：

Limited research has been conducted on the internal tendering procedures (ITP) of construction contractors because of the commercially sensitive and confidential nature of the subject matter. This limitation explains the reluctance of contractors to undergo interviews. Existing research (outside bid/no-bid and margin decision factor identification and subsequent decision modeling development) only begins to provide insights into key tendering stages, particularly around risk assessments and corporate review processes. Early research suggested one to three review stages. However, when considering the whole work procurement process from prospect identification to contract execution, five to seven series of reviews can be arguably applied by some contractors, wherein some reviews stepped through several layers of internal senior management. Tendering processes were presented as flowchart models that traditionally follow “hard” system (rectangular shapes and straight line arrows) steps, which suggest that a precise process also leads to precise results. However, given that contractors do not win every tender they submit, the process is less precise than that suggested in rigidly structured flowcharts. Twenty-five detailed semi-structured interviews were held with purposely selected high-profile publicly and privately owned construction companies in Australia with significantly varied turnovers. Analyses show that contractors are concerned about the negative effects of increasing corporate governance demands, with many stating that people involved are the most critical element to tendering success. A new way of presenting the ITP of contractors is assessed using a soft systems methodology (SSM) approach. SSM offers an alternative way of considering human interaction challenges within the ITP of contractors, which needs to be tested with the industry. The format graphics of SSM guidelines are presented as a way of offering contractors a different approach, which may assist individuals who are looking to re-structure their tendering activities in a more humanistic and less rigid procedural approach.

关键词： contractor     corporate governance     humanistic     risk     soft systems methodology     tendering procedures    

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Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation

Luis A. ALFONSO-HERRERA, Leticia M. TORRES-MARTINEZ, J. Manuel MORA-HERNANDEZ

《能源前沿（英文）》 2022年 第16卷 第5期   页码 734-746 doi: 10.1007/s11708-022-0840-x

摘要： This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal–organic framework (MOF)-based systems toward the photocatalytic hydrogen evolution (PHE) reaction through specific strategies: tailoring the photocatalytic activity of bare MOFs and guest@MOF composites, formation of heterojunctions based on MOFs and various photocatalysts, and inorganic photocatalysts derived from MOFs. According to the data reported in this mini-review, the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units (SBUs). Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view, many of these studies relate this activity to the physicochemical and catalytic properties of MOFs. However, they did not consider the interactions between the components of the photocatalytic material. This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE. A thorough review and comparison of the results established that metal–nanoparticle@MOF composites have weak van der Waals forces between components, whereas heterostructures only interact with MOFs at the surface of bare materials. Regarding material derivatives from MOFs, we found that pyrolysis destroyed some beneficial properties of MOFs for PHE. Thus, we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.

关键词： metal–organic frameworks (MOFs)     photocatalytic hydrogen evolution     MOF heterojunctions     materials derived from MOFs     bandgap     recombination    

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绿色化工应用导向的金属-有机框架材料研究概述 Review

孔祥婧, 李建荣

《工程（英文）》 2021年 第7卷 第8期   页码 1115-1139 doi: 10.1016/j.eng.2021.07.001

摘要：

快速的工业化进程导致当今全球性的能源和环境危机，以推动科技进步、解决相关挑战为目标，发展新型功能材料的重要性与日俱增。近年来，金属-有机框架（MOF）以及MOF衍生物材料引起了广泛关注，促使我们继续进行其结构设计和应用性能方面的探索。MOF材料的制备、表征和加工成型是实现其工业应用的基础。研究人员已经围绕这些主题开展了大量的工作，以绿色化工应用为导向，充分发挥功能性优势，推动MOF材料大规模的工业应用也应当被提上日程。在解决实际问题的过程中，许多经典MOF表现出了相对传统材料的优越性。文中将从MOF化学中的基本概念出发，讨论了MOF材料的工业合成进展及其在多个领域中的应用现状，旨在提供一个系统的研究概述，引导研究者逐渐将研究思路从学术研究转向实际应用。在成本、规模化生产、加工成型和稳定性等挑战被逐一突破之后，MOF及其衍生物材料有望走进工厂，成为我们日常生活中的一部分，进而为人类创造一个基于绿色生产和生活方式的新时代。

关键词： 金属-有机框架     应用     绿色化工    

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标题 作者 时间 类型 操作

Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

期刊论文

Zeolitic imidazolate framework-8 (ZIF-8) for drug delivery: A critical review

Simin Feng, Xiaoli Zhang, Dunyun Shi, Zheng Wang

期刊论文

Cobalt-nanoparticle catalysts derived from zeolitic imidazolate framework@MXene composites for efficient

期刊论文

Parametric study on the mixed solvent synthesis of ZIF-8 nano- and micro-particles for CO adsorption: A response surface study

Alireza Hadi, Javad Karimi-Sabet, Abolfazl Dastbaz

期刊论文

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

期刊论文

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

期刊论文

Metal-organic frameworks for CO

Lei ZHANG, Junqing ZHANG

期刊论文

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction

期刊论文

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

期刊论文

Crystalline porous materials: from zeolites to metal-organic frameworks (MOFs)

Zaiku Xie, Bao-Lian Su

期刊论文

Hierarchical porous metal-organic frameworks/polymer microparticles for enhanced catalytic degradation

期刊论文

Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient

期刊论文

Rethinking the tendering frameworks of construction contractors in the context of a soft systems methodology

Stephen URQUHART, Andrew WHYTE

期刊论文

Novel strategies to tailor the photocatalytic activity of metal–organic frameworks for hydrogen generation

Luis A. ALFONSO-HERRERA, Leticia M. TORRES-MARTINEZ, J. Manuel MORA-HERNANDEZ

期刊论文

绿色化工应用导向的金属-有机框架材料研究概述

孔祥婧, 李建荣

期刊论文