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“Heating where it hurts”: Electromagnetic induction remote energy transfer to a solid catalyst enables waste polymer upcycling "加热痛处":电磁感应远程能量转移到固体催化剂,实现废弃聚合物的再循环利用
Pub Date : 2024-07-25 DOI: 10.1016/j.mtcata.2024.100059
Marcos G. Farpón, Enrique Torregrosa, Gonzalo Prieto

Electromagnetic induction heating currently attracts significant attention as a means to electrify catalytic processes and leverage a highly specific and localized energy supply. This Comment article features the application of this unconventional energy input for waste polymer conversion to fuel hydrocarbons.

目前,电磁感应加热作为催化过程电气化和利用高度特定和局部能源供应的一种手段,备受关注。这篇评论文章介绍了这种非常规能源输入在废聚合物转化为燃料烃过程中的应用。
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引用次数: 0
Investigation of m- and p-xylene linked bimetallic Ni-cyclam-complexes as potential electrocatalysts for the CO2 reduction 研究作为潜在二氧化碳还原电催化剂的间二甲苯和对二甲苯连接双金属镍-环-络合物
Pub Date : 2024-06-23 DOI: 10.1016/j.mtcata.2024.100058
Sarah Bimmermann , Daniel Siegmund , Kallol Ray , Ulf-Peter Apfel

Among the various molecular CO2 reduction catalysts, the [Ni(cyclam)]2+ (Ni-{N4}) complex with its earth-abundant metal center and macrocyclic ligand proved to be efficient for the selective electrochemical conversion of CO2 to CO. In the present study we now connected the two Ni-cyclam units by using para- and meta-xylene as organic linkers attached to the amines of the macrocycle to form the p-{Ni2} and m-{Ni2} complexes, respectively, and test them as catalysts for the electrochemical CO2 reduction reactions. Notably, the p-{Ni2} complex demonstrates a higher faraday efficiency in the electrochemical reduction of CO2 to CO compared to the m-{Ni2} complex. This finding highlights the significant role played by the M-M distance in influencing this catalytic process.

在各种二氧化碳还原分子催化剂中,[Ni(cyclam)]2+(Ni-{N4})配合物以其富集的金属中心和大环配体被证明是将二氧化碳选择性电化学转化为一氧化碳的有效催化剂。在本研究中,我们使用对二甲苯和间二甲苯作为有机连接体,将两个 Ni 环单元连接到大环的胺上,分别形成了 p-{Ni2} 和 m-{Ni2} 复合物,并将它们作为电化学 CO2 还原反应的催化剂进行了测试。值得注意的是,与 m-{Ni2} 复合物相比,p-{Ni2} 复合物在电化学还原 CO2 到 CO 的过程中表现出更高的法拉第效率。这一发现凸显了 M-M 间距在影响这一催化过程中所起的重要作用。
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引用次数: 0
Ediorial Board 编辑委员会
Pub Date : 2024-06-01 DOI: 10.1016/S2949-754X(24)00019-X
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引用次数: 0
Modification strategies and applications of Mn–Cd–S solid solution-based photocatalysts 基于 Mn-Cd-S 固溶体的光催化剂的改性策略和应用
Pub Date : 2024-06-01 DOI: 10.1016/j.mtcata.2024.100055
Songqing Zhang , Jiarui Lou , Chenhui Wang , Qian Li , Yufeng Li , Linfeng Jin , Changfa Guo

Semiconductor photocatalyzed energy production and environment treatment have received a lot of attention. Mn–Cd–S solid solutions (MnxCd1−xS) with tunable band structure, suitable redox capacity, and visible light response is recognized as one of the most promising photocatalysts for practical applications. However, low separation efficiency of photogenerated carriers and sluggish reaction kinetics restricts its photocatalytic activity. This review discusses the advantages and drawbacks of MnxCd1−xS for photocatalysis in terms of electronic band structure and surveys the modification strategies of photocatalytic activity, including modulation of Mn/Cd ratio, morphology/structure regulation, defect engineering, construction of heterojunction, loading cocatalysts, and integration of multiple strategies. Then, the progress in photocatalytic water splitting to hydrogen, carbon dioxide reduction, and pollutant degradation using MnxCd1−xS-based materials are summarized. Finally, it is concluded by outlining the challenges and opportunities for developing efficient photocatalysts based on MnxCd1−xS.

半导体光催化能源生产和环境治理受到广泛关注。锰-镉-S固溶体(MnxCd1-xS)具有可调的带状结构、合适的氧化还原能力和可见光响应,是公认的最有实际应用前景的光催化剂之一。然而,光生载流子的分离效率低和反应动力学迟缓限制了它的光催化活性。本综述讨论了 MnxCd1-xS 在光催化电子能带结构方面的优缺点,并研究了光催化活性的改性策略,包括锰/镉比调控、形貌/结构调控、缺陷工程、异质结构建、负载共催化剂以及多种策略的整合。然后,总结了使用 MnxCd1-xS 基材料在光催化水分离制氢、二氧化碳还原和污染物降解方面的进展。最后,概述了开发基于 MnxCd1-xS 的高效光催化剂所面临的挑战和机遇。
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引用次数: 0
Cover 封面
Pub Date : 2024-06-01 DOI: 10.1016/S2949-754X(24)00018-8
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引用次数: 0
Effect of β-fluorinated porphyrin in changing selectivity for electrochemical O2 reduction β-氟化卟啉对改变电化学氧气还原选择性的影响
Pub Date : 2024-06-01 DOI: 10.1016/j.mtcata.2024.100053
Ashwin Chaturvedi , Sandeep Dash , Soumalya Sinha , Julien A. Panetier , Jianbing Jiang Jimmy

The development of catalytic systems that selectively convert O2 to water is required to progress fuel cell technology. As an alternative to platinum catalysts, derivatives of iron and cobalt porphyrin molecular catalysts provide one benchmark for catalyst design. However, the inclusion of these catalysts into homogeneous platforms remains a difficulty. Co-porphyrins have been studied as heterogeneous O2 reduction catalysts; however, they have not been explored much in homogeneous systems. Moreover, they suffer from poor selectivity for the desired four-electron reduction of O2 to H2O. Herein, we present two cobalt-based β-fluorinated porphyrin complexes (CoTPF8(OH)2 and CoTPF8(OH)4) and demonstrate applicability as effective catalysts for the oxygen reduction reaction. Using rotating ring-disk electrochemistry, the catalysts, CoTPF8(OH)2 and CoTPF8(OH)4, showed maximum Faradaic efficiency for H2O of 92 % and 97 %, respectively. DFT calculations suggest that the formation of a phlorin intermediate could occur before O2 reduction and that a stronger H2O2 binding in the cobalt-based β-fluorinated porphyrin species compared to the unsubstituted parent compound, CoTP(OH)2, was responsible for the observed experimental selectivity for H2O. These results reveal that the β-fluorinated porphyrin catalyst serves as a novel platform for investigating molecular electrocatalytic reactions.

要想推动燃料电池技术的发展,就必须开发出能有选择地将氧气转化为水的催化系统。作为铂催化剂的替代品,铁和钴卟啉分子催化剂的衍生物为催化剂设计提供了一个基准。然而,将这些催化剂纳入均相平台仍是一个难题。人们已经将共卟啉作为异相 O2 还原催化剂进行了研究,但在均相系统中对它们的研究还不多。此外,它们在将 O2 还原成 H2O 的所需四电子选择性较差。在此,我们介绍了两种钴基β-氟化卟啉配合物(CoTPF8(OH)2 和 CoTPF8(OH)4),并证明了它们可作为氧还原反应的有效催化剂。利用旋转环盘电化学原理,CoTPF8(OH)2 和 CoTPF8(OH)4 催化剂对 H2O 的最大法拉第效率分别为 92% 和 97%。DFT 计算表明,在还原 O2 之前可能会形成一个叶绿素中间体,而且与未取代的母体化合物 CoTP(OH)2 相比,钴基β-氟化卟啉物种与 H2O2 的结合力更强,这是观察到的 H2O 实验选择性的原因。这些结果表明,β-氟化卟啉催化剂是研究分子电催化反应的新型平台。
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引用次数: 0
MXene-based catalysts: A review 基于二甲苯的催化剂:综述
Pub Date : 2024-06-01 DOI: 10.1016/j.mtcata.2024.100054
Ali Hamzehlouy , Masoud Soroush

Two-dimensional (2D) materials, such as graphene, hexagonal boron nitride, 2D metal–organic frameworks, layered double hydroxides, transition metal dichalcogenides, and MXenes, have garnered significant attention in catalysis due to their exceptional properties and structures. Notably, recent studies have revealed the promising catalytic activity of MXene-based catalysts for many reactions, including hydrogen evolution, oxygen evolution, oxygen reduction, nitrogen reduction, carbon dioxide reduction, alcohol oxidation, hydrogenation, dehydrogenation, methanol conversion, dry reforming of methane, and CO oxidation. This review offers a summary of recent advances in the field, contextualizing the progress made. Additionally, it delves into existing challenges while presenting prospects for future developments in this domain.

二维(2D)材料,如石墨烯、六方氮化硼、二维金属有机框架、层状双氢氧化物、过渡金属二钙化物和二氧化二烯,因其优异的性能和结构而在催化领域备受关注。值得注意的是,最近的研究揭示了基于 MXene 的催化剂在许多反应中具有良好的催化活性,包括氢进化、氧进化、氧还原、氮还原、二氧化碳还原、醇氧化、氢化、脱氢、甲醇转化、甲烷干重整和 CO 氧化。本综述概述了该领域的最新进展,并对所取得的进展进行了背景分析。此外,它还深入探讨了现有的挑战,并对该领域的未来发展进行了展望。
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引用次数: 0
A review: Simultaneous "one-pot" pollution mitigation and hydrogen production from industrial wastewater using photoelectrocatalysis process 综述:利用光电催化工艺同时从工业废水中 "一锅式 "减少污染和制氢
Pub Date : 2024-05-22 DOI: 10.1016/j.mtcata.2024.100052
Nyiko M. Chauke , Mpfunzeni Raphulu

This review delves into the underlying principles, advantages, challenges, and recent developments in photoelectrocatalysis (PEC) processes for wastewater treatment and green hydrogen production. PEC is an emerging technique that holds great promise for addressing two critical challenges simultaneously, namely, the degradation of industrial wastewater pollutants and the generation of clean energy in the form of hydrogen gas. In recent years, many studies have explored the use of photoanodes to harness solar energy for wastewater treatment. These photoanodes facilitate the breakdown of contaminants, while the cathode concurrently produces green hydrogen. The PEC enables the production of both clean water and hydrogen gas from industrial wastewater. This dual benefit makes it an attractive avenue for sustainable industrial wastewater treatment and clean energy generation. The PEC process capitalizes on the constructive interaction between electrochemical reactions and photocatalysis. Solar energy is efficiently converted into electron-hole pairs, which play a pivotal role in water-splitting reactions occurring at the electrode surfaces. Achieving the best performance involves scrutiny of various parameters, including catalyst loading, pH, light intensity, and electrolyte composition. The photoelectrocatalytic system shows commendable stability and durability during extended operation, reinforcing its practical applicability. This review provides a comprehensive overview of the PEC process, catalyst materials, optimization strategies, and driving efficiency. Considering the potential benefits and costs on a larger scale underscores the significance of photoelectrocatalytic hydrogen production in addressing environmental concerns and energy-related issues concurrently. Therefore, PEC is a promising pathway toward sustainable water treatment and clean energy, bridging the gap between environmental stewardship and technological advancement.

本综述深入探讨了用于废水处理和绿色制氢的光电催化(PEC)工艺的基本原理、优势、挑战和最新发展。光电催化是一种新兴技术,有望同时解决两个关键挑战,即降解工业废水污染物和以氢气形式产生清洁能源。近年来,许多研究都在探索使用光阳极来利用太阳能进行废水处理。这些光阳极可促进污染物的分解,同时阴极可产生绿色氢气。PEC 可以从工业废水中生产清洁水和氢气。这种双重优势使其成为可持续工业废水处理和清洁能源生产的一个极具吸引力的途径。PEC 工艺利用了电化学反应和光催化之间的建设性相互作用。太阳能被有效地转化为电子-空穴对,而电子-空穴对在电极表面发生的水分离反应中起着关键作用。要实现最佳性能,需要对各种参数进行仔细研究,包括催化剂负载、pH 值、光照强度和电解质成分。光电催化系统在长期运行过程中表现出了值得称道的稳定性和耐久性,从而增强了其实际应用性。本综述全面概述了光触媒催化过程、催化剂材料、优化策略和驱动效率。考虑到更大规模的潜在效益和成本,光电催化制氢在同时解决环境问题和能源相关问题方面具有重要意义。因此,光电催化制氢是实现可持续水处理和清洁能源的一条大有可为的途径,在环境管理和技术进步之间架起了一座桥梁。
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引用次数: 0
Highly scalable and robust ribbon-like coordination polymer as green catalyst for Hantzsch condensation in synthesis of DHPs and bioactive drug molecule 高可扩展性和鲁棒性带状配位聚合物作为绿色催化剂用于合成二羟基化合物和生物活性药物分子的汉兹奇缩合反应
Pub Date : 2024-05-12 DOI: 10.1016/j.mtcata.2024.100051
Debolina Mukherjee, Apu Saha, Dipak Basak, Rupam Sahoo, Madhab C. Das

Ribbon-like coordination polymers (CP) represents a highly unexplored innovative class of metal-coordination network. Herein, we have developed a highly scalable and chemically robust (pH = 3–10 stable) ribbon-like CP [{Cu(Pim)(L)(H2O)·H2O}]n (1) following a complete environment-friendly green synthesis route. Considering the presence of surface flanked labile coordinated water molecules and their appealing correlation with one-dimensional structural characteristics, such sort of ribbon-like CP was explored for the first time as excellent heterogeneous surface catalyst for largely unexplored three-component Hantzsch condensation for synthesis of different classes of dihydropyridine (DHP). Moreover, 1 is employed to synthesize bio-responsive drug ‘Ethidine’ (possessing high anti-oxidant and anticarcinogenic properties) characterized with Single Crystal X-ray Diffraction (SCXRD) analysis. Several DHP-based products are also analysed through in-depth SCXRD analysis. This report inaugurates the usage of a Cu(II) based ribbon-like CPs as heterogeneous surface catalyst following environmentally benign manner for synthesis of bioactive DHPs and Drugs.

带状配位聚合物(CP)是一类尚未开发的创新型金属配位网络。在此,我们采用完整的环境友好型绿色合成路线,开发出了一种具有高度可扩展性和化学稳定性(pH = 3-10 稳定)的带状配位聚合物[{Cu(Pim)(L)(H2O)-H2O}]n (1)。考虑到表面侧翼易配位水分子的存在及其与一维结构特征之间的诱人相关性,这种带状 CP 被首次用作优秀的异相表面催化剂,用于合成不同种类的二氢吡啶(DHP),而这种催化剂在很大程度上尚未被用于三组分汉兹奇缩合反应。此外,1 还被用于合成生物反应药物 "乙脒"(具有高度抗氧化和抗癌特性),并通过单晶 X 射线衍射(SCXRD)分析对其进行了表征。报告还通过深入的 SCXRD 分析对几种基于 DHP 的产品进行了分析。本报告开创性地使用基于 Cu(II) 的带状 CPs 作为异相表面催化剂,以对环境无害的方式合成具有生物活性的 DHPs 和药物。
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引用次数: 0
Pore size modulation of cobalt-corrole-based porous organic polymers for boosted electrocatalytic oxygen reduction reaction 调节钴-丙烯醛基多孔有机聚合物的孔径,促进电催化氧还原反应
Pub Date : 2024-04-20 DOI: 10.1016/j.mtcata.2024.100050
Qian Zhao , Qingxin Zhang , Yizhen Wu , Zixuan Xiao , Yuxin Peng , Yuxin Zhou , Wei Zhang , Haitao Lei , Rui Cao

The highly active and selective oxygen reduction reaction (ORR) is vital to promote the performance of advanced energy conversion systems, such as fuel cells and other electrochemical devices. Porous framework materials have the capability to combine the catalytic performance of catalytic active units with their porous characteristics, making them promising oxygen reduction catalysts. However, due to the difficulty in designing and synthesizing catalytic active units, the pore size modulation of framework materials is primarily achieved by altering the linkers. We herein report the design and synthesis of three cobalt-corrole-based porous organic polymers (Co-POP-1, Co-POP-2 and Co-POP-3) with different pore sizes, which were obtained by extending 5,15-meso substituents of Co corroles. Compared to Co-POP-1 and Co-POP-2, Co-POP-3 has the largest pore size. Benefiting from the enhanced mass transfer and the highly exposed active sites, Co-POP-3 displayed remarkably boosted activity for the selective four-electron/four-proton (4e/4 H+) ORR with a half-wave potential of E1/2 = 0.89 V versus reversible hydrogen electrode (RHE) in 0.1 M KOH solutions. This work not only presents a cobalt-corrole-based porous organic polymer catalyst with high ORR activity and selectivity but also provides a new strategy to moderate the pore size of porous framework materials.

高活性和选择性氧还原反应(ORR)对于提高燃料电池和其他电化学装置等先进能源转换系统的性能至关重要。多孔骨架材料能够将催化活性单元的催化性能与其多孔特性结合起来,使其成为前景广阔的氧还原催化剂。然而,由于设计和合成催化活性单元存在困难,框架材料的孔径调节主要是通过改变连接体来实现的。我们在此报告了通过扩展钴的 5,15-介取代基,设计并合成了三种具有不同孔径的钴-科罗拉多基多孔有机聚合物(Co-POP-1、Co-POP-2 和 Co-POP-3)。与 Co-POP-1 和 Co-POP-2 相比,Co-POP-3 的孔径最大。得益于增强的传质和高度暴露的活性位点,Co-POP-3 在 0.1 M KOH 溶液中的选择性四电子/四质子(4e-/4 H+)ORR 活性显著提高,与可逆氢电极(RHE)相比,其半波电位为 E1/2 = 0.89 V。这项研究不仅提出了一种具有高 ORR 活性和选择性的钴-丙烯醛基多孔有机聚合物催化剂,还提供了一种调节多孔框架材料孔径的新策略。
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引用次数: 0
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Materials Today Catalysis
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