ChemSusChem最新文献

{"title":"Small Molecule π-π Stacking Promotes Efficient Photoelectrocatalytic Splitting of Aqueous Hydrogen Production from Polyaniline.","authors":"Weixing Nie, Mengnan Ruan, Chengyi Wang, Zhifeng Liu","doi":"10.1002/cssc.202401363","DOIUrl":"10.1002/cssc.202401363","url":null,"abstract":"<p><p>Photoelectrocatalysis efficiency depends on light absorption and the effective use of photogenerated carriers but is often limited by inefficient charge transfer and catalytic surface reactivity. In this study, π-π stacking of polar small molecules on aromatic ring-rich polyaniline (PANI) was carried out to improve its photoelectrocatalytic splitting of water for hydrogen production. Detailed photoelectrochemical experiments and density-functional theory (DFT) calculations show that small molecules of p-aminobenzoic acid (PABA) and PANI have the best π-π stacking (compared to p-toluenesulfonic acid (PTA)), which promotes the separation of carriers on the PANI surface. In addition, the polar effect of the small molecules also improves the reactivity of the PANI surface and also reduces the potential barrier for H₂ evolution. The current density of PANI-PABA reached -0.12 mA/cm² (1.23 V vs. RHE) 2.53 times higher than that of pure PANI in linear voltammetric scanning tests under light. This strategy of introducing polar small molecules into organocatalysts via π-π stacking will provide new ideas for the preparation of efficient organic photoelectrocatalysis.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401363"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142046028","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}

{"title":"Enzymatic Degradation of PFAS: Current Status and Ongoing Challenges.","authors":"Benjamin A Harris, Jinpeng Zhou, Bradley O Clarke, Ivanhoe K H Leung","doi":"10.1002/cssc.202401122","DOIUrl":"10.1002/cssc.202401122","url":null,"abstract":"<p><p>Per- and polyfluoroalkyl substances (PFAS) are often considered the quintessential example of industrial chemical pollution - they are toxic and ubiquitous environmental contaminants that are extremely difficult to degrade. There has been a large research focus on the development of effective and renewable degradation technologies. In comparison to traditional pollutant degradation techniques, such as advanced oxidation processes and electrochemistry, degradation of PFAS using extracellular enzymes offers an eco-friendly solution as enzymes are biodegradable, recyclable and have low energy and chemical requirements. This review outlines the current understanding of extracellular enzymatic degradation of PFAS with a focus on reported results and proposed degradation mechanisms. More importantly, this review highlights limitations that hinder the application of enzymes for PFAS degradation and proposes critical future research that is needed to improve the applicability of this promising remediation strategy.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401122"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11739852/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141986919","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Recycling and Reutilization of Metals Aided by Deep Eutectic Solvents: from NMC Cathodes of Spent Li-ion Batteries to Electrolytes for Supercapacitors.","authors":"Boren Xu, Noel Díez, Marta Sevilla, María L Ferrer, María C Gutiérrez, Francisco Del Monte","doi":"10.1002/cssc.202401128","DOIUrl":"10.1002/cssc.202401128","url":null,"abstract":"<p><p>With the rapidly increasing demand for lithium ion batteries (LIBs), recycling the metals found in spent cathodes is mandatory to both alleviate shortages resulting from the mining of natural metal ores and manage the disposal of spent LIBs. The use of deep eutectic solvents (DESs) for metals recovery from spent cathodes of LIBs (e. g., LCO and NMC types) offers a sustainable yet efficient alternative to conventional hydrometallurgical processes. Nonetheless, g efforts are required to use milder temperatures and higher mass loadings, thus ensuring cost-effectiveness. In this latter regard, addressing the reutilization of DESs in subsequent stages of metal extraction, and streamlining or eliminating the chemical procedures employed for metal separation, is even more crucial to guarantee the economic feasibility of the recycling process. Herein, we have prepared a DES that provides extraction efficiencies of ca. 100 % for every metal of NMC cathodes even at mild experimental conditions (e. g., 60 °C) and for loadings as high as 70 mg_NMC/g_DES. Moreover, we have pioneered the direct use of leachates containing DESs and metals as electrolytes for supercapacitors. This approach enables the reintroduction of DESs and the recovered metals into the value chain with a minimal economic and environmental impact.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401128"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11739843/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141764581","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"s-scheme3D/3D Bi⁰/BiOBr/P Doped g-C3 N4 with Oxygen Vacancies (Ov) for Photodegradation of Pharmaceuticals: In-situ H₂O₂ Production and Plasmon Induced Stability.","authors":"Mope E Malefane, Muthumuni Managa, Thabo T I Nkambule, Alex T Kuvarega","doi":"10.1002/cssc.202401471","DOIUrl":"10.1002/cssc.202401471","url":null,"abstract":"<p><p>Complications accompanying photocatalyst stability and recombination of exciton charges in pollutants degradation has been addressed through the construction of heterojunctions, especially S-scheme heterojunction with strong and distinctive redox centres. Herein, an S-scheme BiOBr (BOR) and g-C₃N₄PO₄ (CNPO) catalyst (BORCNPO) with oxygen vacancy (Ov) was synthesized for levofloxacin (LVX) and oxytetracycline (OTC) photodegradation under visible light. The 3D/3D BORCNPO catalyst possessed C-O-Br bridging bonds for efficient charge transfer during the fabrication of S-scheme heterojunction. In-situ H₂O₂ formation affirmed by potassium titanium (IV) oxalate spectrophotometric method improved the mineralization ability of BORCNPO7.5 catalyst. Bi⁰ surface plasmon resonance (SPR) enhanced formation and involvement of ⋅O₂ ^- and the stability of the catalyst which increased reaction rate with increasing cycling experiments. XPS and radical trapping experiments supported the S-scheme charge transfer mechanism formation with high degradation rate of LVX which was 3 times higher than OTC degradation rate. Mineralization of pollutants and their intermediates were demonstrated with florescence excitation and emission matrix (FEEM) and quadruple time of flight high performance liquid chromatography (QTOF-HPLC). This work advances development of highly stable and efficient catalysts for photodegradation of pollutants through the formation of S-scheme heterostructure.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401471"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11739848/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141986921","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"FeNi-LDH Coated With Orange-Peel Carbon Aerogel for Oxygen Evolution Reaction.","authors":"Yang Teng, Peng-Cheng Ji, Hai-Lang Jia","doi":"10.1002/cssc.202401276","DOIUrl":"10.1002/cssc.202401276","url":null,"abstract":"<p><p>In this work, the waste orange-peel was used as carbon source, and the orange-peel derived carbon material can be obtained through simple pyrolysis. Then, we designed the structure of orange-peel carbon aerogel grown on iron-nickel layered double hydroxides in situ to achieve the effect of carbon coating (FeNi-LDH/CA). The oxygen evolution reaction catalytic performance of FeNi-LDH/CA is excellent, far exceeding that of commercial RuO₂. In 1 M KOH, the overpotential of FeNi-LDH/CA is only 250 mV (10 mA cm^-2), obviously better than that of commercial RuO₂ (295 mV). FeNi-LDH/CA shows good cycling stability, and after long-term i-t testing, the performance only decays by 3 % after running at 100 mA cm^-2 for 100 h. When used as an anode, the voltage of water-splitting is only 1.48 V at 10 mA cm^-2. The rechargeable liquid zinc-air battery based on Pt/C-FeNi-LDH/CA catalyst has higher open-circuit voltage (1.543 V) and galvanostatic discharge capacity at 1.23 V (830 min, 10 mA cm^-2). Moreover, the zinc-air battery based on Pt/C-FeNi-LDH/CA has a small charge-discharge voltage gap (0.65 V) at 10 mA cm^-2, after 200 consecutive cycles (66 h), the charge-discharge voltage gap only increased by about 30 mV, indicating good cycling stability.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401276"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141755965","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}

{"title":"Synergistic Regulation of Sodium Metal Deposition Pattern Through Three-Dimensional Sodiophilic Gradient ZnO/Fe_0.7Co_0.3 Frameworks and Magnetic Fields for High-Performance Sodium Metal Batteries.","authors":"Yunfei Wang, Yuanhao Wang, Xiang Sun, Wenhua Yang, Jie Xu, Derang Cao, Shandong Li, Xia Wang","doi":"10.1002/cssc.202400675","DOIUrl":"10.1002/cssc.202400675","url":null,"abstract":"<p><p>The application of sodium metal battery is hampered by the large volume change and uncontrollable top growth of Na metal. Herein, a dual strategy including constructing a three-dimensional gradient ZnO/Fe_0.7Co_0.3 (ZFC) framework of decreasing sodiophilic capability from bottom to top, and imposing magnetic fields based on magnetohydrodynamic (MHD) effect, is proposed to regulate the sodium deposition/stripping behavior and realize the bottom-up deposition of Na. Therefore, the ZFC framework under a magnetic field of 200 mT exhibits high electrochemical reversibility with a Coulombic efficiency of 99.77 % at 1 mA cm^-2 and 1 mAh cm^-2. Meanwhile, the ZFC composite anode (ZFC@Na) with the magnetic field of 200 mT delivers a small polarization voltage of approximately10 mV and long cycle life of more than 2500 h at 5 mA cm^-2 and 5 mAh cm^-2 in symmetric cells, along with good cycle stability in ZFC@Na||Na₃V₂(PO₄)₃ full cells (200 cycles at 1 C with a high capacity retention of 98 %). Accordingly, the novel strategy of combining magnetic fields and sodiophilic gradient frameworks provides a perspective to solve the issues of sodium dendrite growth.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400675"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141755897","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}

{"title":"Design and Synthesis of Sb-Doped CuS@C Hollow Nanocubes as Efficient Anode Materials for Sodium-Ion Battery.","authors":"Xiang Zheng, Zining Zhang, Zhiqian Li, Chaohong Shi, Jianqing Zhao, Jing Tang","doi":"10.1002/cssc.202401271","DOIUrl":"10.1002/cssc.202401271","url":null,"abstract":"<p><p>Copper sulfide has received widespread attention for application as anode materials in sodium-ion batteries due to their potent capabilitiess and eco-friendly properties. However, it is a challenge to achieve a high rate capability and long cycle stability owing to the heterogeneous transfer of sodium ions during charge-discharge, the interior poor electron conductivity and repeated volumetric expansion of copper sulfide. In this study, Sb-doped copper sulfide hollow nanocubes coated with carbon shells (Sb-CuS@C) was designed and constructed as anode nanomaterials in sodium-ion batteries. Thanks to the intrinsic good electron conductivity and chemical stability of carbon shells, Sb-CuS@C possesses a higher overall electron transfer as anode material, avoids agglomeration and structural destruction during the cycling. As a result, the synthesized Sb-CuS@C achieved an excellent reversible capacity of 595 mA h g^-1 after 100 cycles at 0.5 A g^-1 and a good rate capability of 340 mA h g^-1 at a higher 10 A g^-1. DFT calculations clarify that the uniformly doped Sb would act as active sodiophilic nucleation sites to help adsorbing sodium-ion during discharging and leading uniform sodium deposition. This work provides a new insight into the structural and componential modification for common transition-metal sulfides towards application as anode materials in sodium-ion battery.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401271"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141858443","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}

{"title":"Ultra-Dilute SnCl₄-Catalyzed Conversion of Concentrated Glucose to 5-Hydroxymethylfurfural in Aqueous Deep Eutectic Solvent.","authors":"Guo Xusheng, Qin Chuan, Si Yuxi, Lyu Xilei, Cheng Youwei","doi":"10.1002/cssc.202401105","DOIUrl":"10.1002/cssc.202401105","url":null,"abstract":"<p><p>5-Hydroxymethylfurfural(HMF) is a versatile chemical synthesized from glucose dehydration catalyzed by metal chloride (MCl_x) in deep eutectic solvents (DESs). However, the low glucose concentration and high catalyst dosage hinder large-scale HMF production. Herein, we report an aqueous DES of tetraethylammonium bromide(TEAB)-glucose for converting concentrated glucose (40 wt %, relative to TEAB) using ultra-dilute SnCl₄ (0.25 mol %), achieving a 62 % yield of HMF. Ultra-dilute MCl_x-catalyzed selective conversion of glucose is feasible only when combining SnCl₄ with Br-based DES, which is elucidated by density functional theory and molecular dynamic calculations. Using SnCl₄ is essential due to its higher glucose isomerization activity than AlCl₃ and CrCl₃, which can be attributed to its low-barrier coordination with glucose and its barrier-free separation from fructose. Halide anions in DESs strongly interact with glucose, hindering the MCl_x-glucose coordination and thereby reducing MCl_x's activity for glucose isomerization. Consequently, Br-based DESs facilitate higher activity of MCl_x than Cl-based DESs, due to the weaker interaction between halide anion and glucose. In addition, we elucidated the side reactions including condensation, polymerization, and isomerization, and proposed a reaction network. Our findings clarify the differential activity of MCl_x and the impact of halide anions in DESs on MCl_x's activity.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401105"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141873674","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}

{"title":"High-Performance Sodium-Ion Batteries with Graphene: An Overview of Recent Developments and Design.","authors":"Sachin Sharma Ashok Kumar, M Nujud Badawi, J Liew, Thibeorchews Prasankumar, K Ramesh, S Ramesh, S Ramesh, S K Tiong","doi":"10.1002/cssc.202400958","DOIUrl":"10.1002/cssc.202400958","url":null,"abstract":"<p><p>Due to their low production cost, sodium-ion batteries (SIBs) are considered attractive alternatives to lithium-ion batteries (LIBs) for next generation sustainable and large-scale energy storage systems. However, during the charge/discharge cycle, a large volume strain is resulted due to the presence of a large radius of sodium ions and high molar compared to lithium ions, which further leads to poor cyclic stability and lower reversible capacity. In the past, researchers have devoted significant efforts to explore various anode materials to achieve SIBs with high energy density. Hence, as a promising anode material for SIBs, the two-dimensional (2D) materials including graphene and its derivatives and metal oxides have attracted remarkable attention due to their layered structure and superior physical and chemical properties. The inclusion of graphene and metal oxides with other nanomaterials in electrodes have led to the significant enhancements in electrical conductivity, reaction kinetics, capacity, rate performance and accommodating the large volume change respectively. Moreover, these 2D materials facilitated large surface areas and shorter paths for sodium ion adsorption and transportation respectively. In this review article, the fabrication techniques, structural configuration, sodium ion storage mechanism and its electrochemical performances will be introduced. Subsequently, an insight into the recent advancements in SIBs associated with 2D anode materials (graphene, graphene oxide (GO), transition metal oxides etc.) and other graphene-like elementary analogues (germanene, stanine etc.) as anode materials respectively will be discussed. Finally, the key challenges and future perspectives of SIBs towards enhancing the sodium storage performance of graphene-based electrode materials are discussed. In summary, we believe that this review will shed light on the path towards achieving long-cycling life, low operation cost and safe SIBs with high energy density using 2D anode materials and to be suitably commercialized for large-scale energy storage applications in the future.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202400958"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141974621","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}

{"title":"Selective Lithium Recovery from Spent Lithium Manganate Batteries Using Oxidative Stabilization Technique.","authors":"Yong Yan, Ming Zhang, Zhi-Jie Zhang, Shan Ma, Min Chen, Dan Zhou, Lei Sun, Haibin Cheng, Zhi Chen, Cong-Ming Tang, Jun-Qiang Xu","doi":"10.1002/cssc.202401289","DOIUrl":"10.1002/cssc.202401289","url":null,"abstract":"<p><p>Using oxidizing compounds to handle the recycling of discarded lithium batteries has advanced significantly in recent years. One of the most prominent methods is the sintered electrode powder treatment using pre-used additives, with an aqueous solution of the oxidizing agent fueling highly selective lithium extraction and transition metals retention in the refractory material. Herein, phosphoric acid (H₃PO₄) was used as the exchanger and hydrogen ions provider, the oxidant (K₂S₂O₈) activity was driven by heating, the raw material structure was deformed and adjusted by the oxidizing drive, and lithium was exhausted, while manganese was converted into manganese(III) phosphate hydrate and manganese dioxide insoluble material. The optimized conditions resulted in a lithium leaching rate of 94.16 % and a separation factor of 95.74 %, while the corresponding manganese leaching rate was limited to less than 5 %. The X-ray diffraction, X-ray spectroscopy, scanning electron microscopy, and inductively coupled plasma mass spectrometry measurements were used to investigate the influence of oxidation driving force and lithium leaching. Finally, the lithium leach solution was continuously stirred with sodium carbonate in boiling water to obtain the precipitate, which was separated and washed several times to obtain high-purity lithium carbonate.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e202401289"},"PeriodicalIF":7.5,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141910927","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}