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Selective Degradation of Polyethylene Terephthalate Plastic Waste Using Iron Salt Photocatalysts. 利用铁盐光催化剂选择性降解聚对苯二甲酸乙二醇酯塑料废料。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-06 DOI: 10.1002/cssc.202401920
Shusheng Jiang, Miao Wang, Yahao Huang, Jinglan Wen, Peng Hu

Plastic pollution poses a significant challenge to environmental conservation. Efficient recycling of plastic is a key strategy to address this issue. Polyethylene terephthalate (PET), commonly found in plastic bottles, represents a substantial portion of plastic waste. Consequently, the efficient degradation and recycling of PET is crucial for the sustainable development of society. However, the implementation of methods for PET depolymerization and recycling typically necessitates alkaline/acidic pre-treatment and significant energy input for heating. Here, we propose a gentle, and highly efficient photocatalysis approach for selectively degrading PET plastic waste into terephthalic acid (TPA) in high yield (up to 99%) using cost-effective iron salts. Notably, this method achieved excellent selectivity with high TON and TOF values, applying oxygen or air as environmentally friendly oxidants. In addition, the solvent can be recycled without compromising the TPA yield, and large-scale reactions can be performed smoothly.

塑料污染对环境保护构成了重大挑战。高效回收塑料是解决这一问题的关键策略。塑料瓶中常见的聚对苯二甲酸乙二醇酯(PET)占塑料垃圾的很大一部分。因此,有效降解和回收 PET 对社会的可持续发展至关重要。然而,PET 解聚和回收方法的实施通常需要碱/酸预处理和大量的加热能源投入。在此,我们提出了一种温和、高效的光催化方法,利用具有成本效益的铁盐选择性地将 PET 塑料废料高产率(高达 99%)降解为对苯二甲酸(TPA)。值得注意的是,这种方法在使用氧气或空气作为环保氧化剂的情况下,实现了极佳的选择性和较高的 TON 值和 TOF 值。此外,溶剂可以循环使用,而不会影响 TPA 收率,大规模反应也能顺利进行。
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引用次数: 0
Sustainable Hydrogen Production by Glycerol and Monosaccharides Catalytic Acceptorless Dehydrogenation (AD) in Homogeneous Phase. 在均相中利用甘油和单糖催化无受体脱氢 (AD) 实现可持续制氢。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-06 DOI: 10.1002/cssc.202400639
Sylwia Kostera, Luca Gonsalvi

In the quest for sustainable hydrogen production, the use of biomass-derived feedstock is gaining importance. Acceptorless Dehydrogenation (AD) in the presence of efficient and selective catalysts has been explored worldwide as a suitable method to produce hydrogen from hydrogen-rich simple organic molecules. Among these, glycerol and sugars have the advantage of being cheap, abundant, and obtainable from fatty acid basic hydrolysis (biodiesel industry) and from biomass by biochemical and thermochemical processing, respectively. Although heterogeneous catalysts are more widely used for hydrogen production from biomass-based feedstock, the harsh reaction conditions applied limit applicability due to deactivation of active sites due to coking  of carbonaceous materials. Moreover, heterogeneous catalyst are more difficult to fine-tune than homogeneous counterparts, and the latter also allow for high process selectivities under milder conditions. The present Concept article summarizes the main features of the most active homogeneous catalysts reported for glycerol and monosaccharides AD. In order to directly compare  hydrogen production efficiencies, the choice of literature works was limited to reports where hydrogen was clearly quantified by yields and turnover numbers (TONs). The types of transition metals and ligands is discussed, together with a perspective view on future challenges of homogeneous AD reactions for practical applications.

在寻求可持续制氢的过程中,生物质原料的使用正变得越来越重要。在高效和选择性催化剂的作用下,无受体脱氢(AD)作为一种从富氢简单有机分子制氢的合适方法,已在全球范围内得到探索。其中,甘油和糖具有廉价、丰富的优势,可分别从脂肪酸基础水解(生物柴油工业)和生物质中通过生化和热化学处理获得。虽然异相催化剂更广泛地用于以生物质为原料制氢,但由于碳质材料结焦导致活性位点失活,因此苛刻的反应条件限制了其适用性。此外,与均相催化剂相比,异相催化剂更难进行微调,而均相催化剂还能在较温和的条件下实现较高的工艺选择性。本概念文章总结了已报道的用于甘油和单糖 AD 的最活跃均相催化剂的主要特点。为了直接比较制氢效率,对文献作品的选择仅限于通过产率和周转次数(TONs)对氢进行明确量化的报告。本文讨论了过渡金属和配体的类型,并展望了均相 AD 反应在实际应用中的未来挑战。
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引用次数: 0
CORRIGENDUM: Correction to Solid State Zinc and Aluminum Ion Batteries: Challenges and Opportunities. 更正:更正为 "固态锌和铝离子电池:挑战与机遇。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-06 DOI: 10.1002/cssc.202401926
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引用次数: 0
Cation Vacancy-Mediated Ultrafast Hole Transport in CuBi2O4 Photocathodes. CuBi2O4 光阴极中阳离子空位介导的超快空穴传输。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-06 DOI: 10.1002/cssc.202401345
Emir Ardalı, Hadi Jahangiri, Navid Solati, Ugur Yahsi, Cumali Tav, Alphan Sennaroglu, Sarp Kaya

In this study, the ultrafast transport dynamics of the valence band hole states in CuBi2O4 (CBO) photocathodes were investigated by varying the atomic composition and manipulating their p-type character. As a comprehensive ultrafast optical transient absorption spectroscopy (TAS) investigation of compositionally manipulated CBO that combines both ex situ and in situ TAS experiments with photoelectrochemical (PEC) performance tests, the study reveals the polaron formation tendencies of the valence band (VB) holes at cationic vacancy sites. Therefore, it draws a complete picture of the ultrafast hole transport dynamics and provides valuable insights into the hindrance of the photocurrent generated in CBO.

本研究通过改变 CuBi2O4(CBO)光电阴极的原子成分并操纵其 p 型特性,研究了其价带空穴态的超快传输动力学。该研究结合了原位和非原位瞬态吸收光谱实验以及光电化学(PEC)性能测试,是对经过成分处理的 CBO 进行的一次全面的超快光学瞬态吸收光谱(TAS)研究,揭示了阳离子空位处价带(VB)空穴的极子形成趋势。因此,它描绘了超快空穴传输动力学的全貌,并为了解 CBO 中产生的光电流的阻碍因素提供了宝贵的见解。
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引用次数: 0
Selective Modification of the Product Profile of Biocatalytic Hydrolyzed PET via Product-specific Medium Engineering. 通过产品特异性培养基工程选择性修改生物催化水解 PET 的产品谱。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-06 DOI: 10.1002/cssc.202401759
Tobias Heinks, Katrin Hofmann, Simon Last, Igor Gamm, Luise Blach, Ren Wei, Uwe T Bornscheuer, Christof Hamel, Jan von Langermann

Over the past years, enzymatic depolymerization of PET, one of the most widely used plastics worldwide, has become very efficient leading to the end products terephthalic acid (TPA) and ethylene glycol (EG) used for PET re-synthesis. Potent alternatives to these monomers are the intermediates BHET and MHET, the mono- and di-esters of TPA and EG which avoid total hydrolysis and can serve as single starting materials for direct re-polymerization. This study therefore aimed to selectively prepare those intermediates through reaction medium engineering during the biocatalytic hydrolysis of PET. After a comparative pre-screening of 12 PET-hydrolyzing enzymes, two of them (LCCICCG, IsPETasewt) were chosen for detailed investigations. Depending on the reaction conditions, MHET and BHET are predominantly obtainable: (i) MHET was produced in a better ratio and high concentrations at the beginning of the reaction when IsPETasewt and 10% EG was used; (ii) BHET was produced as predominant product when LCCICCG and 25% EG was used. TPA itself was nearly the single product at pH 9.0 after 24 h due to the self-hydrolysis of MHET and BHET under basic conditions. Using medium engineering in biocatalytic PET-hydrolysis, the product profile can be adjusted so that TPA, MHET or BHET is predominantly produced.

聚对苯二甲酸(TPA)和乙二醇(EG)是全球使用最广泛的塑料之一,在过去几年中,聚对苯二甲酸(PET)的酶解效率非常高,最终产品对苯二甲酸(TPA)和乙二醇(EG)被用于聚对苯二甲酸(PET)的再合成。这些单体的有效替代品是中间体 BHET 和 MHET,它们是 TPA 和 EG 的单酯和二酯,可避免完全水解,并可作为直接再聚合的单一起始原料。因此,本研究旨在通过反应介质工程,在 PET 的生物催化水解过程中选择性地制备这些中间体。在对 12 种 PET水解酶进行比较预筛选后,选择了其中两种(LCCICCG 和 IsPETasewt)进行详细研究。根据反应条件的不同,可主要获得 MHET 和 BHET:(i) 使用 IsPETasewt 和 10% EG 时,MHET 的生成比例较好,且在反应初期浓度较高;(ii) 使用 LCCICCG 和 25% EG 时,BHET 成为主要生成物。由于 MHET 和 BHET 在碱性条件下会发生自水解,因此 24 小时后,在 pH 值为 9.0 时,TPA 本身几乎是唯一的产物。在生物催化 PET- 水解过程中使用培养基工程技术,可以调整产物分布,使 TPA、MHET 或 BHET 成为主要产物。
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引用次数: 0
Electrocatalysts for the Formation of Hydrogen Peroxide by Oxygen Reduction Reaction. 通过氧还原反应生成过氧化氢的电催化剂。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-06 DOI: 10.1002/cssc.202401952
Ke Yuan, Hong Li, Xindi Gu, Yalei Zheng, Xiaodong Wu, Yihe Zhao, Jiejie Zhou, Sheng Cui

Hydrogen peroxide (H2O2) is a widely used strong oxidant, and its traditional preparation methods, anthraquinone method, and direct synthesis method, have many drawbacks. The method of producing H2O2 by two-electron oxygen reduction reaction (2e- ORR) is considered an alternative strategy for the traditional anthraquinone method due to its high efficiency, energy saving, and environmental friendliness, but it remains a big challenge. In this review, we have described the mechanism of ORR and the principle of electrocatalytic performance testing, and have summarized the standard performance evaluation techniques for electrocatalysts to produce H2O2. Secondly, according to the theoretical calculation and experimental results, several kinds of efficient electrocatalysts are introduced. It is concluded that noble metal-based materials, carbon-based materials, non-noble metal composites, and single-atom catalysts are the preferred catalyst materials for the preparation of H2O2 by 2e- ORR. Finally, the advantages and novelty of 2e- ORR compared with traditional methods for H2O2 production, as well as the advantages and disadvantages of the above-mentioned high-efficiency catalysts, are summarized. The application prospect and development direction of high-efficiency catalysts for H2O2 production by 2e- ORR has been prospected, which is of great significance for promoting the electrochemical yield of H2O2 and developing green chemical production.

过氧化氢(H2O2)是一种广泛使用的强氧化剂,其传统的制备方法--蒽醌法和直接合成法--存在许多缺点。通过双电子氧还原反应(2e- ORR)制备 H2O2 的方法因其高效、节能、环保而被认为是传统蒽醌法的替代策略,但它仍然是一个巨大的挑战。在这篇综述中,我们阐述了 ORR 的机理和电催化性能测试的原理,总结了产生 H2O2 的电催化剂的标准性能评估技术。其次,根据理论计算和实验结果,介绍了几种高效电催化剂。结论是贵金属基材料、碳基材料、非贵金属复合材料和单原子催化剂是 2e- ORR 制备 H2O2 的首选催化剂材料。最后,总结了 2e- ORR 与传统 H2O2 生产方法相比的优势和新颖性,以及上述高效催化剂的优缺点。展望了 2e- ORR 产 H2O2 高效催化剂的应用前景和发展方向,对提高 H2O2 电化学产率和发展绿色化工生产具有重要意义。
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引用次数: 0
An Efficient Cathode Catalyst for Rechargeable Zinc-air Batteries based on the Derivatives of MXene@ZIFs. 基于 MXene@ZIFs 衍生物的可充电锌-空气电池高效阴极催化剂。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401200
Fei Zhao, Li Kang, Jilan Long, Keyu Chen, Simeng Ding

Oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are crucial processes at the cathode of zinc-air batteries. Developing highly efficient and durable electrocatalysts at the air cathode is significant for the practical application of rechargeable zinc-air batteries. Herein, N-doped layered MX containing Co2P/Ni2P nanoparticles is synthesized by growing CoNi-ZIF on the surface and interlayers of the two-dimensional material MXene (Ti2C3) followed by phosphating calcination. The growth of CoNi-ZIF on the surface of MXene results in the attenuation of high-temperature structural damage of MXene, which in turn leads to the formation of Co2P/Ni2P@MX with a hierarchical configuration, higher electron conductivity, and abundant active sites. The optimized Co2P/Ni2P@MX achieves a half-wave potential of 0.85 V for the ORR and an overpotential of 345 mV for the OER. In addition, DFT calculations were adopted to investigate the mechanism at the atomic and molecular levels. The liquid zinc-air battery with Co2P/Ni2P@MX as the cathode exhibits a specific capacity of 783.7 mAh g-1 and exceeds 280 h (840 cycles) cycle stability, superior to zinc-air batteries constructed by the cathode of commercial Pt/C+RuO2 and other previous works. Furthermore, a solid-state battery synthesized with Co2P/Ni2P@MX as the cathode exhibits stable cycle performance (154 h/462 cycles).

氧还原反应(ORR)和氧进化反应(OER)是锌-空气电池阴极的关键过程。开发高效耐用的空气阴极电催化剂对于锌-空气充电电池的实际应用意义重大。本文通过在二维材料 MXene(Ti2C3)的表面和夹层上生长 CoNi-ZIF 并进行磷化煅烧,合成了含有 Co2P/Ni2P 纳米颗粒的 N 掺杂层状 MX。CoNi-ZIF 在 MXene 表面的生长减弱了 MXene 的高温结构损伤,进而形成了具有分层构型、更高电子传导性和丰富活性位点的 Co2P/Ni2P@MX。优化后的 Co2P/Ni2P@MX 在 ORR 中的半波电位为 0.85 V,在 OER 中的过电位为 345 mV。此外,还采用 DFT 计算研究了原子和分子水平的机理。以 Co2P/Ni2P@MX 为阴极的液态锌-空气电池的比容量为 783.7 mAh g-1,循环稳定性超过 280 h(840 次),优于以商用 Pt/C+RuO2 为阴极构建的锌-空气电池和其他先前的研究成果。此外,用 Co2P/Ni2P@MX 作为阴极合成的固态电池具有稳定的循环性能(154 小时/462 次循环)。
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引用次数: 0
Trace Iron-Modified CeO₂-supported Core-shell CoO@Co Catalyst for Selective Conversion of Furfural to 1,5-Pentanediol. 微量铁改性 CeO₂支撑的核壳 CoO@Co 催化剂用于糠醛到 1,5-Pentanediol 的选择性转化。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401938
Shenyu Wang, Junjie Zhang, Ying Zhang

In the conversion of furfural using non-noble metal catalysts, preferential cleavage of the C2-O bond followed by hydrogenation of the C=C bond facilitates selective access to valuable 1,5-pentanediol (1,5-Ped). Herein, we developed CeO₂ loaded core-shell CoO@Co nanoparticle catalysts. Adjusting Co loading, Fe doping, and reduction temperature improved reaction efficiency. 7Co-0.2Fe/CeO₂ catalysts reduced at 500 °C demonstrated optimal performance. 1,5-Ped produced at 54.76 mmol/g(Co)/h, representing the top activity levels among the reported catalysts. H₂-TPR, XRD, HAADF-STEM, FT-IR, XPS, and XANES were employed to investigate the catalyst structure-activity relationship. Co²⁺ cleaves furan ring C-O bond, Co⁰ promotes double-bond hydrogenation. The CoO@Co structure favors the desired 1,5-Ped production route. Trace Fe species optimize the Co²⁺/Co⁰ ratio, enhance the substrate adsorption, and inhibit the furan ring saturation. These findings emphasize the importance of fine-tuning catalyst structure and composition for selectivity improvement.

在使用非贵金属催化剂进行糠醛转化时,C2-O 键的优先裂解和 C=C 键的氢化有助于选择性地获得有价值的 1,5-pentanediol (1,5-Ped)。在此,我们开发了负载 CeO₂ 的核壳 CoO@Co 纳米粒子催化剂。调整钴负载、铁掺杂和还原温度可提高反应效率。在 500 °C 下还原的 7Co-0.2Fe/CeO₂ 催化剂表现出最佳性能。1,5-Ped 的生产率为 54.76 mmol/g(Co)/h,在已报道的催化剂中活性最高。为了研究催化剂结构与活性之间的关系,采用了 H₂-TPR、XRD、HAADF-STEM、FT-IR、XPS 和 XANES 等方法。Co²⁺ 裂解呋喃环上的 C-O 键,Co⁰ 促进双键氢化。CoO@Co 结构有利于理想的 1,5-Ped 生产路线。微量铁元素优化了 Co²⁺/Co⁰ 的比例,增强了对底物的吸附,抑制了呋喃环的饱和。这些发现强调了微调催化剂结构和组成对提高选择性的重要性。
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引用次数: 0
Purification of Li2CO3 obtained through pyrometallurgical treatment of NMC black mass from electric vehicle batteries. 通过火法冶金处理电动汽车电池中的 NMC 黑质,提纯 Li2CO3。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401722
Rosso Laura, Alcaraz Lorena, Rodríguez-Largo Olga, Félix López

The recycling of lithium batteries is essential for a sustainable energy transition. However, impurities in the products obtained from the black mass can lower their market value. In this work, lithium carbonate, which has the highest market share among lithium-based products, is purified using distilled water at controlled temperature, time and stirring speed. The purification process involves dissolving lithium carbonate in distilled water at low temperatures (between 0 and 10°C), followed by crystallization through water evaporation. Optimal conditions yielded lithium carbonate with a purity of 99.66% after two stages of purification. The dependence of the variables on the final purity was deeply analyzed and the thermodynamics of the reaction was studied, confirming the exothermic nature the dissolution reaction.

锂电池的回收利用对于可持续能源转型至关重要。然而,从黑块中获得的产品中的杂质会降低其市场价值。在这项工作中,使用蒸馏水在可控温度、时间和搅拌速度下对锂基产品中市场份额最高的碳酸锂进行提纯。纯化过程包括在低温(0 至 10°C)下将碳酸锂溶解在蒸馏水中,然后通过水蒸发结晶。经过两个阶段的提纯,最佳条件下得到的碳酸锂纯度为 99.66%。研究人员深入分析了各变量对最终纯度的影响,并对反应的热力学进行了研究,证实了溶解反应的放热性质。
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引用次数: 0
Z-Scheme Enabled 1D/2D Nanocomposite of ZnO Nanorods and Functionalized g-C3 N4 Nanosheets for Sustainable Degradation of Terephthalic Acid. Z-Scheme Enabled 1D/2D Nanocomposite of ZnO Nanorods and Functionalized g-C3 N4 Nanosheets for Sustainable Degradation of Terephthalic Acid(Z-Scheme Enabled 1D/2D Nanocomposite of ZnO Nanorods and Functionalized g-C3 N4 Nanosheets)。
IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401408
Honey Mittal, Arun Kumar, Diksha Sharma, Manika Khanuja

The urgent need to mitigate water pollution and achieve Sustainable Development Goal 14 (SDG 14)-Life below water, necessitates developing efficient and eco-friendly wastewater treatment technologies. This research addresses this challenge by photocatalytic degradation of terephthalic acid, a precursor for PET bottles using environment-friendly and biocompatible photocatalysts. The 1D/2D nanocomposite comprising zinc oxide (ZnO) nanorods and functionalized graphitic carbon nitride (Zn-TG) nanosheets were synthesized and thoroughly characterized. The nanocomposite effectively mitigated the individual drawbacks of Zn-TG agglomeration and the wide band gap of ZnO as confirmed through zeta potential and Tauc's plot studies, respectively. The synthesized nanocomposite achieved ~100 % degradation within 60 minutes, exhibiting superior kinetics (~2.5 times) compared to pristine samples. The enhanced degradation efficiency was elucidated by efficient charge carrier transfer (~5 times faster) and separation (~2 times improved) as confirmed through electrochemical impedance spectroscopy and time-resolved photoluminescence studies. The proposed Z-scheme pathway provides mechanistic insights. This proposed mechanism is supported by extensive electron paramagnetic resonance (EPR) and scavenger studies. The liquid chromatography-mass spectrometry (LC-MS) analysis confirms the formation of less toxic byproducts for ensuring that the wastewater treatment process is efficient and environmentally friendly. This research helps in developing a highly effective and sustainable wastewater treatment technology.

减轻水污染和实现可持续发展目标 14(SDG 14)--"生活在水深火热之中 "的迫切需要要求开发高效、生态友好的废水处理技术。本研究利用环境友好、生物兼容的光催化剂对 PET 瓶的前体对苯二甲酸进行光催化降解,从而应对这一挑战。研究人员合成了由氧化锌(ZnO)纳米棒和功能化氮化石墨碳(Zn-TG)纳米片组成的 1D/2D 纳米复合材料,并对其进行了全面表征。该纳米复合材料有效地缓解了 Zn-TG 团聚和氧化锌带隙过宽的缺点,ZETA 电位和陶氏图谱研究分别证实了这一点。与原始样品相比,合成的纳米复合材料在 60 分钟内实现了 ~100% 的降解,表现出更优越的动力学性能(~2.5 倍)。电化学阻抗光谱和时间分辨光致发光研究证实,高效的电荷载流子转移(约快 5 倍)和分离(约提高 2 倍)提高了降解效率。提出的 Z 方案途径提供了机理上的启示。广泛的电子顺磁共振(EPR)和清除剂研究为这一拟议机制提供了支持。液相色谱-质谱(LC-MS)分析确认了毒性较低的副产品的形成,从而确保了废水处理过程的高效性和环保性。这项研究有助于开发一种高效、可持续的废水处理技术。
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引用次数: 0
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