ChemSusChem最新文献_第7页

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

ChemSusChem Pub Date : 2024-11-06 DOI: 10.1002/cssc.202400639

Sylwia Kostera, Luca Gonsalvi

{"title":"Sustainable Hydrogen Production by Glycerol and Monosaccharides Catalytic Acceptorless Dehydrogenation (AD) in Homogeneous Phase.","authors":"Sylwia Kostera, Luca Gonsalvi","doi":"10.1002/cssc.202400639","DOIUrl":"https://doi.org/10.1002/cssc.202400639","url":null,"abstract":"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.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400639"},"PeriodicalIF":7.5,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581206","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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

ChemSusChem Pub Date : 2024-11-06 DOI: 10.1002/cssc.202401345

Emir Ardalı, Hadi Jahangiri, Navid Solati, Ugur Yahsi, Cumali Tav, Alphan Sennaroglu, Sarp Kaya

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

ChemSusChem 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

{"title":"Selective Modification of the Product Profile of Biocatalytic Hydrolyzed PET via Product-Specific Medium Engineering.","authors":"Tobias Heinks, Katrin Hofmann, Simon Last, Igor Gamm, Luise Blach, Ren Wei, Uwe T Bornscheuer, Christof Hamel, Jan von Langermann","doi":"10.1002/cssc.202401759","DOIUrl":"10.1002/cssc.202401759","url":null,"abstract":"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.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401759"},"PeriodicalIF":7.5,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589668","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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

ChemSusChem 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

{"title":"Electrocatalysts for the Formation of Hydrogen Peroxide by Oxygen Reduction Reaction.","authors":"Ke Yuan, Hong Li, Xindi Gu, Yalei Zheng, Xiaodong Wu, Yihe Zhao, Jiejie Zhou, Sheng Cui","doi":"10.1002/cssc.202401952","DOIUrl":"10.1002/cssc.202401952","url":null,"abstract":"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.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401952"},"PeriodicalIF":7.5,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581100","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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

ChemSusChem Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401200

Fei Zhao, Li Kang, Jilan Long, Keyu Chen, Simeng Ding

{"title":"An Efficient Cathode Catalyst for Rechargeable Zinc-air Batteries based on the Derivatives of MXene@ZIFs.","authors":"Fei Zhao, Li Kang, Jilan Long, Keyu Chen, Simeng Ding","doi":"10.1002/cssc.202401200","DOIUrl":"https://doi.org/10.1002/cssc.202401200","url":null,"abstract":"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).","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401200"},"PeriodicalIF":7.5,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581055","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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

ChemSusChem Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401938

Shenyu Wang, Junjie Zhang, Ying Zhang

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

ChemSusChem Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401722

Laura Rosso, Lorena Alcaraz, Olga Rodríguez-Largo, Félix A López

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

ChemSusChem Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401408

Honey Mittal, Arun Kumar, Diksha Sharma, Manika Khanuja

{"title":"Z-Scheme Enabled 1D/2D Nanocomposite of ZnO Nanorods and Functionalized g-C3 N4 Nanosheets for Sustainable Degradation of Terephthalic Acid.","authors":"Honey Mittal, Arun Kumar, Diksha Sharma, Manika Khanuja","doi":"10.1002/cssc.202401408","DOIUrl":"https://doi.org/10.1002/cssc.202401408","url":null,"abstract":"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.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401408"},"PeriodicalIF":7.5,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581216","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Application of Hydroxyaromatic Aldehydes in Ultra-Efficient and Metal-Free Photocatalytic E→Z Isomerization of Olefin. 羟基芳醛在超高效无金属光催化 E→Z 烯烃异构化中的应用。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-05 DOI: 10.1002/cssc.202401387

Chun-Xiu Liu, Yao Yao, Zi-Wen Zhou, Song Qin, Zhi-Peng Yu, Fei-Yan Tao, Wen-Dian Li, Xiao-Qi Yu, Na Wang

{"title":"Application of Hydroxyaromatic Aldehydes in Ultra-Efficient and Metal-Free Photocatalytic E→Z Isomerization of Olefin.","authors":"Chun-Xiu Liu, Yao Yao, Zi-Wen Zhou, Song Qin, Zhi-Peng Yu, Fei-Yan Tao, Wen-Dian Li, Xiao-Qi Yu, Na Wang","doi":"10.1002/cssc.202401387","DOIUrl":"https://doi.org/10.1002/cssc.202401387","url":null,"abstract":"The strategy of photocatalyzed E→Z isomerization of olefins to access thermodynamically less stable Z-alkenes has recently received considerable attention. Here, we have discovered a sensitizer of hydroxyaromatic aldehyde that can rapidly achieve olefin E→Z isomerization under blue light irradiation. Notably, 2-hydroxybenzene-1,3,5-tricarbaldehyde, when assisted by blue light, can achieve efficient and selective conversion within just 5 minutes (Z/E=92 : 8). The reaction can be successfully scaled up to gram scale, and exhibits remarkable reactivity toward various derivatives of ethyl cinnamate (27 examples) and other olefins. Furthermore, the former can be directly cyclized by a hydroxyl derivative to produce 4-substituted coumarin. The prominent preponderance of this method includes being metal-free, efficient, convenient, no by-products and achieving high selectivity. Correlation of sensitizer triplet energy (ET) and preliminary mechanistic experiments indicate that the accomplishment of this reaction is based on the selective excitation mechanism.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401387"},"PeriodicalIF":7.5,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Mechanistic Insights on Coverage-Dependent Selectivity Limitations in Vinyl Acetate Synthesis. 乙酸乙烯酯合成中覆盖层选择性限制的机理认识。

IF 7.5 2区化学

ChemSusChem Pub Date : 2024-11-03 DOI: 10.1002/cssc.202401911

Gregory L Novotny, Prashant Deshlahra

{"title":"Mechanistic Insights on Coverage-Dependent Selectivity Limitations in Vinyl Acetate Synthesis.","authors":"Gregory L Novotny, Prashant Deshlahra","doi":"10.1002/cssc.202401911","DOIUrl":"10.1002/cssc.202401911","url":null,"abstract":"Developing improved catalysts for sustainable chemical processes often involves understanding atomistic origins of catalytic activity, selectivity, and stability. Using density functional theory and steady-state kinetic analyses, we probe the elementary steps that form decomposition products that limit selectivity in vinyl acetate (VA) synthesis on Pd surfaces covered with acetate species. Acetate formation and coupling with ethylene control the VA formation catalytic cycle and steady-state coverage, but acetate and ethylene can separately decompose to form CO2. Both decompositions involve initial C-H activations at acetate vacancies, followed by additional C-H activations and eventual C-O formations and C-C cleavages involving reactions with molecular oxygen. Acetate decomposition paths with non-oxidative kinetically-relevant steps exhibit similar free energy barriers to oxidative paths. In contrast, the non-oxidative ethylene path involving an ethylidyne intermediate exhibits a much lower barrier than paths with oxidative kinetically-relevant steps. Ethylene decomposition is very facile at low coverages but is more coverage-sensitive, leading to similar decomposition and VA formation barriers at coverages accessible at steady state, which is consistent with moderate VA selectivity in measurements and ethylene vs. acetate decomposition contributions assessed from regressed kinetic parameters. These insights provide a detailed framework for describing VA synthesis rates and selectivity on metallic catalyst surfaces.","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401911"},"PeriodicalIF":7.5,"publicationDate":"2024-11-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142566782","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0