ChemSusChem最新文献

{"title":"Reductive Catalytic Fractionation of Lignocellulosic Biomass: The Impact of Impurities in Catalyst.","authors":"Yiping Zhu, Haiyun Huang, Haibin Gou, Shuaihao Sun, Yuhe Liao","doi":"10.1002/cssc.202500199","DOIUrl":"10.1002/cssc.202500199","url":null,"abstract":"<p><p>Catalytic fractionation of lignocellulosic biomass is a promising technology for obtaining different fractions and the valorization of lignin. Reductive catalytic fractionation (RCF) is one of these technologies in which catalysts play an essential role. In this work, the impact of impurities in catalysts on the output of RCF is investigated. It is found that the yield of phenolic monomers is almost not influenced by the residual chloride (Cl) ions in the commercially available Ru/C catalyst. However, the presence of Cl ions in the catalyst facilitated hemicellulose removal and delignification. Moreover, the enzymatic conversion rate of cellulose in the solid residue increases after RCF, attributed to the enhanced removal of lignin and hemicellulose in the presence of Cl ions. The impact of Cl ions can be eliminated by removing the Cl ions in the catalyst. This work provides an engineering perspective for upscaling RCF technology using large-scale synthesized catalysts.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500199"},"PeriodicalIF":7.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143954203","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":"Synthesis of Lithium Manganese Oxide and Ti-Substituted LMO Sorbents for Lithium Extraction in a Spray-Drying Process.","authors":"Laura Herrmann, Nicole Bohn, Alisa Pfau, Thomas Kölbel, Helmut Ehrenberg, Joachim R Binder, Fabian Jeschull","doi":"10.1002/cssc.202500530","DOIUrl":"10.1002/cssc.202500530","url":null,"abstract":"<p><p>Lithium manganese oxides (LMO) are highly promising sorbents for lithium extraction from Li <math> <semantics> <mrow><msup><mrow></mrow> <mo>+</mo></msup> </mrow> <annotation>$^{&#x00026;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;plus;}$</annotation></semantics> </math> -containing brines with high salt contents due to their high sorption capacity and high selectivity toward lithium. However, conventional synthesis routes are limited in scale. Therefore, a novel spray-drying method is presented herein, enabling a scalable synthesis of LMO sorbents for Li <math> <semantics> <mrow><msup><mrow></mrow> <mo>+</mo></msup> </mrow> <annotation>$^{&#x00026;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;amp;plus;}$</annotation></semantics> </math> extraction. The ion-exchange material is studied in both synthetic LiCl solutions and two different geothermal brines from the Upper Rhine Valley, demonstrating improved Li selectivity and extraction capabilities compared to materials from hydrothermal synthesis approaches. The extraction behavior in relevant mildly acidic environments is studied in detail. Further material improvements are achieved by substituting a fraction of Mn by Ti, which greatly reduced the dissolution of manganese during acid treatment in the first 5 extraction cycles from 5.6% to only 1.8%. In addition, the maximum sorption capacity of the Ti-substituted LMO (LMTO) can be further increased from 5.05 mmol g <math> <semantics> <mrow><msup><mrow></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msup> </mrow> <annotation>$^{- 1}$</annotation></semantics> </math> for LMO (35.1 mg g <math> <semantics> <mrow><msup><mrow></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msup> </mrow> <annotation>$^{- 1}$</annotation></semantics> </math> ) to 5.66 mmol g <math> <semantics> <mrow><msup><mrow></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msup> </mrow> <annotation>$^{- 1}$</annotation></semantics> </math> for LMTO (39.3 mg g <math> <semantics> <mrow><msup><mrow></mrow> <mrow><mo>-</mo> <mn>1</mn></mrow> </msup> </mrow> <annotation>$^{- 1}$</annotation></semantics> </math> ) under optimized m/V ratios. Hence, the results reported herein present a pathway toward LMO-based ion-exchange materials for the direct lithium extraction on an industrial scale.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500530"},"PeriodicalIF":7.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143959117","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":"Mg Plating in Nonethereal Electrolyte Solutions: Fact or Misconception?","authors":"Toshihiko Mandai","doi":"10.1002/cssc.202500418","DOIUrl":"https://doi.org/10.1002/cssc.202500418","url":null,"abstract":"<p><p>Rechargeable Mg metal batteries (RMMBs) have garnered significant attention due to their outstanding electrochemical energy storage performance. Ether solvents are widely used as a primary component of RMMB electrolytes because of their excellent compatibility with Mg metal. However, the poor anodic stability of ethers hinders the development of high-energy-density RMMBs. To address this limitation, researchers have explored novel electrolyte formulations based on nonethereal solvents. However, the interpretation of reported results remains controversial due to a lack of solid experimental evidence confirming Mg plating reactions in such media. This article provides an overview of Mg electrochemistry in both ethereal and nonethereal electrolyte systems. Comprehensive cyclic voltammetry studies on the electrochemical Mg plating/stripping activity in various electrolyte systems reaffirm that only a limited range of solvents-including ethers, amines, and dialkylsulfones-support reversible Mg plating/stripping. In contrast, Mg plating is rarely observed in nitrile, amide, carbonate, and phosphate electrolytes, despite voltammograms exhibiting seemingly reversible responses. These findings caution researchers against assuming voltammetric responses correspond to Mg plating/stripping without solid evidence of Mg deposits. Finally, a protocol for assessing whether proposed (uncommon) electrolyte systems genuinely support Mg plating/stripping is presented.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500418"},"PeriodicalIF":7.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143959915","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":"<ArticleTitle xmlns:ns0=\"http://www.w3.org/1998/Math/MathML\">In Silico Studies Show that -OBO Units Bound to Stable Boron Cages in <ns0:math> <ns0:semantics><ns0:mrow><ns0:mi>Y</ns0:mi> <ns0:msub><ns0:mi>B</ns0:mi> <ns0:mn>11</ns0:mn></ns0:msub> <ns0:msubsup><ns0:mrow><ns0:mo>(</ns0:mo> <ns0:mi>O</ns0:mi> <ns0:mi>B</ns0:mi> <ns0:mi>O</ns0:mi> <ns0:mo>)</ns0:mo></ns0:mrow> <ns0:mn>12</ns0:mn> <ns0:mo>-</ns0:mo></ns0:msubsup> </ns0:mrow> <ns0:annotation>$$ mathbf{Y} {mathbf{B}}_{11} ( mathbf{O} mathbf{B} mathbf{O} {)}_{12}^{-} $$</ns0:annotation></ns0:semantics> </ns0:math> (Y = C/Si) Anions Provide a Desirable Borate-Rich Solid Electrolyte Interface in Ca-Ion Batteries.","authors":"Abhiruchi Sharma, Puneet Gupta","doi":"10.1002/cssc.202500154","DOIUrl":"https://doi.org/10.1002/cssc.202500154","url":null,"abstract":"<p><p>The development of calcium-ion batteries (CIBs) as potential successors to lithium-ion batteries has been hindered by the lack of suitable electrolytes. Conventional electrolytes often decompose on the Ca anode, forming calcium-ion impermeable passivation layers that impede reversible calcium plating and stripping. Therefore, the design of stable electrolytes or those capable of forming Ca²⁺ permeable passivation layers remains a critical challenge. The present study investigates calcium salts of <math> <semantics> <mrow> <msub><mrow><mtext>YB</mtext></mrow> <mrow><mn>11</mn></mrow> </msub> <msubsup><mi>X</mi> <mrow><mn>12</mn></mrow> <mo>-</mo></msubsup> </mrow> <annotation>$left(text{YB}right)_{11} text{X}_{12}^{-}$</annotation></semantics> </math> (Y = C/Si and X = -BO/OBO) anions using density functional theory (DFT)-based simulations for CIBs. DFT calculations emphasize the oxidative stability of anions, while ab initio molecular dynamics (AIMD) simulations reveal their reductive behavior on the Ca anode. Time-dependent charge transfer analysis and projected density of states provide an atomistic perspective on electron transfer between the Ca surface and anions, aligning with observations from frontier orbital analyses. Decomposition of <math> <semantics> <mrow> <msub><mrow><mtext>YB</mtext></mrow> <mrow><mn>11</mn></mrow> </msub> <msubsup> <mrow><mrow><mo>(</mo> <mrow><mtext>OBO</mtext></mrow> <mo>)</mo></mrow> </mrow> <mrow><mn>12</mn></mrow> <mo>-</mo></msubsup> </mrow> <annotation>$left(text{YB}right)_{11} left(left(right. text{OBO} left.right)right)_{12}^{-}$</annotation></semantics> </math> (Y = C/Si) anions during AIMD simulation reveals the formation of borate-based species as part of the solid electrolyte interface, suggesting their potential as electrolytes that enable effective calcium plating and stripping. Overall, this work paves the way for designing efficient electrolytes, offering a fresh perspective to identify optimal CIB electrolytes, and moving beyond ensuring electrolyte stability on the Ca anode.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500154"},"PeriodicalIF":7.5,"publicationDate":"2025-04-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143954667","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":"Converting New Zealand Slash into S-Doped Electrode Materials for High-Performance Supercapacitors.","authors":"Muge Ding, Wei Gao, Shanghai Wei","doi":"10.1002/cssc.202500396","DOIUrl":"https://doi.org/10.1002/cssc.202500396","url":null,"abstract":"<p><p>Slash is a waste product generated from commercial forestry operations. In 2022, flooding slash caused devastating damage when Cyclone Gabrielle directly impacted the Hawke's Bay region of New Zealand. This study addresses the dual challenges of waste management and sustainable materials development by converting forestry slash into high-performance carbon electrodes through an innovative in situ sulfur doping process. Building upon prior research involving waste-derived materials, this study develops a hydrothermal sulfurization technique that transforms New Zealand slash into sulfur-doped, highly graphitized carbon materials with excellent energy storage properties. The hydrothermally sulfurized slash-derived electrode material (C-HS-New Zealand Slash (NZS)) exhibits a high specific capacitance of 148 F g^- ¹ at a current density of 0.5 A g^- ¹. A supercapacitor device assembles with the C-HS-NZS electrode achieves a capacitance of 440 F g^- ¹ at the same current density. The energy density reaches 15.3 Wh kg^- ¹ at a power density of 250 W kg^- ¹. Furthermore, the C-HS-NZS-based device delivers a maximum capacitance of 384 F g^- ¹ and retains 360 F g^- ¹ after 10,000 cycles, demonstrating excellent capacity retention and long-term electrochemical stability.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500396"},"PeriodicalIF":7.5,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143958813","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":"Transient Absorption Microscopy Explores the Effect of Pt Deposition on Charge Carrier Dynamics in Individual Carbon Nitride Particles.","authors":"Sutripto Khasnabis, Cassandra Mesburis, Robert Godin","doi":"10.1002/cssc.202500203","DOIUrl":"https://doi.org/10.1002/cssc.202500203","url":null,"abstract":"<p><p>This study aims to spatially understand the effect of Pt deposition on slow (μs-s) carrier dynamics in carbon nitride (CN_x) photocatalysts, using a homebuilt microsecond diffuse reflectance transient absorption microscopy setup. It is found that Pt deposition lengthens the overall charge half-lives about threefold, while having a spatial preference for binding with respect to defects that induce charge trapping in the μs-s timescale. The initial trapped charge population shows a slight decrease after Pt deposition, suggesting that the more reactive and mobile charges are extracted by Pt sites, leaving behind deeply trapped and long-lived charges. The results emphasize that spatial heterogeneity of surface cocatalysts likely plays a major role in controlling the charge carrier dynamics and activity of photocatalysts.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500203"},"PeriodicalIF":7.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143956530","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":"Interplay between Structure and Conduction Mechanism of Piperazinium-Functionalized Poly[Ethylene Pyrrole/Ethylene Ketone/Propylene Ketone] Anion Conducting Membranes.","authors":"Afaaf Rahat Alvi, Keti Vezzù, Francesco Lanero, Paolo Sgarbossa, Angeloclaudio Nale, Vito Di Noto","doi":"10.1002/cssc.202402765","DOIUrl":"https://doi.org/10.1002/cssc.202402765","url":null,"abstract":"<p><p>Anion exchange membranes (AEMs) have been proposed as potential alternatives to proton exchange membranes in electrochemical energy conversion and storage devices. Herein, the synthesis of a series of AEMs based on random piperazinium-methyl N-substituted poly[ethylene pyrrole/ethylene ketone/propylene ketone] (P-FPKK) and their structural characterization together with the elucidation of the ion conduction mechanism are reported. Different copolymers are prepared by a Paal-Knorr reaction of a poly(ethylene ketone/propylene ketone) copolymer precursor with 1-(2-aminoethyl) piperazine, modulating the molar ratios amine/(1,4-diketonic repeat units of copolymer) from ¼ to 3. The composition and structure are investigated by elemental analysis, attenuated total reflectance-Fourier transform infrared spectroscopy, nuclear magnetic resonance, and X-ray diffraction. The degree of functionalization, f, plays a crucial role in controlling the thermal, morphological, and electrochemical properties of the P-FPKK_f(I)_g and P-FPKK_f(OH)_g membranes. P-FPKK_0.49(OH)_0.45 displays an ionic conductivity of 11.3 mS cm^-1 at 60 °C. After alkaline aging (1 m KOH at 60 °C for 336 h), retaining its structural integrity and 25% of its initial ionic conductivity value, suggesting them as possible candidates for testing in alkaline energy conversion and storage devices. Furthermore, broadband electrical spectroscopy studies reveal that the long-range charge migration processes are modulated by the segmental motion of the backbone chains of the copolymer matrix.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2402765"},"PeriodicalIF":7.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143960633","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":"Additive Engineering Toward Suppression of Sn²⁺ Oxidation in Sn-Pb Perovskite Solar Cells: Mechanisms, Advances, and Outlook.","authors":"Shuo Jiao, Tao Wang, Zhongmin Zhou","doi":"10.1002/cssc.202500333","DOIUrl":"https://doi.org/10.1002/cssc.202500333","url":null,"abstract":"<p><p>Inorganic hybrid tin-lead mixed perovskite solar cells (Sn-Pb PSCs) have attracted widespread attention in virtues of adjustable/narrow bandgaps, low toxicity, and application prospects in all-perovskite tandem solar cells, and the recorded power conversion efficiency (PCE) has reached 24.1%. However, the easy oxidation of Sn²⁺ brings about abundant Sn vacancies and high concentrations of p-type self-doping, leading to the efficiency and durability of Sn-Pb PSCs still lagging behind those of Pb-based counterparts. To inhibit the oxidation of Sn²⁺, feasible additive engineering is proposed and shows impressive effects. Herein, the recent research progress about additive engineering for Pb-Sn PSCs in depth is discussed and reviewed. The additive molecules are classified into antioxidant additives, reducing additives, and competitive additives, according to different action objects, namely Sn²⁺, Sn⁴⁺, and oxygen. Meanwhile, the corresponding functional groups, antioxidant properties, the effect on optoelectronic performances of the device, as well as underlying mechanisms are systematically summarized. Finally, an outlook is provided for future directions in additive engineering toward the suppression of Sn²⁺ oxidation in Sn-Pb perovskites.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2500333"},"PeriodicalIF":7.5,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143958807","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":"The Support can Disguise the Catalytic Effect: The Case of Silver on Alumina in Plasma Ammonia Synthesis.","authors":"Francesco Spadoni, Sofia Perina, Gaia Castellani, Paolo Tosi, Paolo Fornasiero, Vincenzo M Sglavo, Luca Matteo Martini","doi":"10.1002/cssc.202402778","DOIUrl":"https://doi.org/10.1002/cssc.202402778","url":null,"abstract":"<p><p>Plasma catalysis combines the high-energy chemistry of plasma with the speed and selectivity of chemical reactions in catalysis. However, unlike well-established thermal catalysis, a better understanding of fundamental mechanisms is needed, as evidenced by the contrasting results reported in the literature. One main challenge is that not only the genuine catalytic effect may play a role, but both the support and the catalyst also impact the plasma, complicating the understanding. In this study, exploring the impact of support by comparing a single metal on various substrates made of the same material is focused on. Herein, silver on γ-alumina is used to investigate ammonia synthesis in N₂/H₂ plasma discharges. Beyond confirming the beneficial role of silver in ammonia formation, it is also found that the influence of support is crucial and it is affected by the preparation method. These findings contribute to clarifying the discrepancies in the literature results despite using the same materials.</p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":" ","pages":"e2402778"},"PeriodicalIF":7.5,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951660","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":"Front Cover: Rutile-Phase Sn-Ti Mixed Oxides as Acid Catalysts for the Condensation of C2-C3 Oxygenated Compounds in Water (ChemSusChem 8/2025)","authors":"A. Fernández-Arroyo,&nbsp;Marcelo E. Domine","doi":"10.1002/cssc.202580801","DOIUrl":"https://doi.org/10.1002/cssc.202580801","url":null,"abstract":"<p><b>The Front Cover</b> illustrates an innovative approach towards the valorization of aqueous side-streams in biorefineries. Light oxygenated compounds in these complex aqueous effluents are condensed over water-resistant Sn-Ti mixed oxides into hydrocarbons and aromatics under moderate process conditions. These catalysts show a robust rutile phase with hydrophobic characteristics and optimized acid properties, based on Lewis acid sites. The artwork symbolizes how heavier products spontaneously form an upper organic phase layer that can be further processed into biofuels. More information can be found in the Research Article by A. Fernández-Arroyo and M. E. Domine (DOI: 10.1002/cssc.202401761). Cover design: M. L. Martínez.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":149,"journal":{"name":"ChemSusChem","volume":"18 8","pages":""},"PeriodicalIF":7.5,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cssc.202580801","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143831464","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}