Faraday Discussions最新文献_第10页

Charging dynamics of angstrom-scale pores of MXene electrodes with ionic-liquid electrolytes. 离子-液体电解质MXene电极埃级孔的充电动力学。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d5fd00151j

Ming Chen, Sebastian Ostoja-Petkowski, Alexei A Kornyshev

{"title":"Charging dynamics of angstrom-scale pores of MXene electrodes with ionic-liquid electrolytes.","authors":"Ming Chen, Sebastian Ostoja-Petkowski, Alexei A Kornyshev","doi":"10.1039/d5fd00151j","DOIUrl":"10.1039/d5fd00151j","url":null,"abstract":"Transition-metal carbides, MXenes, with angstrom-narrow slit pores are promising electrodes for high-power energy storage, particularly interesting when used with non-volatile ionic-liquid electrolytes. Yet pore charging of such slits remains challenging. Here, we investigate the charging dynamics of ultrathin MXenes immersed in ionic liquid using constant-potential molecular dynamics simulations. Contrary to the prevailing view that the charging process is governed predominantly by pore size, our results uncover a voltage-regulated shift of kinetic control: at low polarization, the charging time is limited mainly by geometric confinement, whereas at high polarization, the relaxation becomes dictated by the applied voltage itself. By introducing the time-resolved charging parameter, we reveal that charging is inherently collective and dynamic, rather than a simple monotonic ion accumulation. The concomitant non-monotonic change in in-pore conductivity further substantiates this picture, reflecting a sequence of voltage-driven structural transitions-from ionic crowding, to field-induced disorder, and finally to a highly packed ionic layer under strong electric fields. Our study unravels the fine details within the picture of angstrom-scale MXene charging dynamics, crucial for understanding the performance of MXene-based supercapacitors.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"131-149"},"PeriodicalIF":3.1,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Charge localization, rectification, and transport in electrolyte patchy nanochannels. 电解质斑块纳米通道中的电荷定位、整流和传输。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d6fd00007j

Sergi G Leyva, Gabriele Dalla Valle, Tine Curk, Ignacio Pagonabarraga

{"title":"Charge localization, rectification, and transport in electrolyte patchy nanochannels.","authors":"Sergi G Leyva, Gabriele Dalla Valle, Tine Curk, Ignacio Pagonabarraga","doi":"10.1039/d6fd00007j","DOIUrl":"10.1039/d6fd00007j","url":null,"abstract":"We study ionic charge localization and transport in electrolyte-filled nanochannels with heterogeneous walls. Localized charged patches at the channel boundaries trap counterions, enabling controlled charge accumulation in otherwise straight channels. Combining lattice-Boltzmann simulations with analytical modeling, we show that the stability and mobility of these charge clouds result from a balance between electrostatic forces, hydrodynamic drag, and diffusion. Under applied electric fields and pressure gradients, localized charge produces diode-like rectification. Pressure-driven flow shifts the dissociation threshold of the counterion cloud, yielding strongly asymmetric current-voltage characteristics. A minimal force-balance model quantitatively captures the rectification window and its linear dependence on the pressure gradient, demonstrating rectification in the absence of geometric asymmetry. We further examine dynamic control using moving wall patches. In the linear electrostatic regime, charge responds diffusively to patch motion, while strong wall potentials induce a strong colocalization and active charge transport. We identify drift- and diffusion-dominated transport regimes and a critical patch velocity beyond which charge localization fails. These results establish patchy wall potentials as a minimal mechanism for controlling ionic localization, rectification, and transport in nanochannels.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"289-308"},"PeriodicalIF":3.1,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148395371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Stimuli-responsive flows in angstrom-scale channels: general discussion. 埃级通道中的刺激响应流：一般讨论。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d6fd90017h

Narayana R Aluru, Mihail Barboiu, Lydéric Bocquet, Marie-Laure Bocquet, Lingzhi Cao, Paola Carbone, Raman Dhiman, Robert A W Dryfe, Michael Fröba, Eden Gage, Abdulghani Ismail, Manu Jaiswal, Tim M Kamsma, Nikita Kavokine, Ayse Saliha Korkut, Manish Kumar, Chong Liu, Jefferson Z Liu, Angelos Michaelides, Andy Mount, Aleksandr Noy, Ignacio Pagonabarraga, Aditya Shivaji Patwari, Susan Perkin, Lauriane Pierrot Deseilligny, Aleksandra Radenovic, Kalyan Raidongia, Khushwant Singh, Zuzanna S Siwy, Daria Turculet, Yongkang Wang, Yanbo Xie, Yujia Zhang

引用次数: 0

Speciation and hydration forces in sodium carbonate/bicarbonate aqueous solutions nanoconfined between mica sheets. 纳米云母片之间碳酸钠/碳酸氢钠水溶液的形态和水合力。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d5fd00145e

Daria Turculet, Shurui Miao, Kieran J Agg, Susan Perkin

{"title":"Speciation and hydration forces in sodium carbonate/bicarbonate aqueous solutions nanoconfined between mica sheets.","authors":"Daria Turculet, Shurui Miao, Kieran J Agg, Susan Perkin","doi":"10.1039/d5fd00145e","DOIUrl":"10.1039/d5fd00145e","url":null,"abstract":"The equilibrium between hydrated and hydrolysed forms of CO2 in water is central to a multitude of processes in geology, oceanography and biology. Chemistry of the carbonate system is well understood in bulk solution, however processes such as mineral weathering and biomineralisation frequently occur in nano-confined spaces where carbonate chemistry is less explored. For confined systems, the speciation equilibria are expected to tilt due to surface reactivity, electric fields and reduced configurational entropy. In this discussion paper we provide measurements of interaction force between negatively charged aluminosilicate (mica) sheets across aqueous carbonate/bicarbonate solutions confined to nanoscale films in equilibrium with a reservoir of the solution. By fitting the measurements to a Poisson-Boltzmann equation modified to account for charge regulation at the bounding walls, we discuss features of the bicarbonate speciation in confinement. We find that (i) the presence of bicarbonate in the bulk reservoir causes a repulsive excess pressure in the slit compared to pH-neutral salt solutions at the same concentration, arising from a higher (negative) effective charge on the mica surfaces; (ii) the electrostatic screening length is lower for solutions of Na2CO3 compared to NaHCO3 at the same bulk concentration, due to a shift in the speciation equilibria with pH and in accordance with Debye-Hückel theory; (iii) hydration forces are observed at distances below 2 nm with features of size 0.1 nm and 0.3 nm; this was reproducible across the various bicarbonate electrolytes studied, and contrasts with hydration forces of uniform step size measured in pH-neutral electrolytes.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"261-273"},"PeriodicalIF":3.1,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13130180/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Molecular and ion sieving with angstrom-channels: general discussion. 用埃通道进行分子和离子筛分：一般讨论。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d6fd90018f

Xavier R Advincula, Narayana R Aluru, Mihail Barboiu, Hélène Berthoumieux, Lydéric Bocquet, Marie-Laure Bocquet, Ming Chen, Raman Dhiman, Aida Fica, Zachary A H Goodwin, Francois Henn, Cecilia Herrero, Tim M Kamsma, Nikita Kavokine, Ayse Saliha Korkut, Alexei A Kornyshev, Manish Kumar, Jefferson Zhe Liu, Angelos Michaelides, Andy Mount, Aleksandr Noy, Sebastian Ostoja-Petkowski, Aleksandra Radenovic, Savannah Silva, René van Roij, Yanbo Xie, Shu Yang

引用次数: 0

When is nanoconfined water different from interfacial water? 纳米承压水与界面水有何不同？

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d5fd00165j

Xavier R Advincula, Christoph Schran, Angelos Michaelides

{"title":"When is nanoconfined water different from interfacial water?","authors":"Xavier R Advincula, Christoph Schran, Angelos Michaelides","doi":"10.1039/d5fd00165j","DOIUrl":"10.1039/d5fd00165j","url":null,"abstract":"Water behaves very differently at surfaces and under extreme confinement, but the boundary between these two regimes has remained unclear. Despite evidence that interfacial effects persist under sub-nanometre confinement, the molecular-scale behaviour and its evolution with slit width remain unclear. Here, we use machine-learning molecular dynamics with first-principles accuracy to probe water at graphene surfaces across slit widths ranging from the open-interface limit to angstrom-scale confinement. We find that water undergoes a sharp structural transition: when three or more water layers fit between the walls, the structure of the graphene-water interface is effectively indistinguishable from that in an open system, with density layering, hydrogen bonding, and orientational ordering retaining interfacial character. Below this threshold, however, angstrom-scale confinement strongly reorganises the liquid, producing enhanced ordering, a restructured hydrogen-bond network, and modified orientational motifs. These results establish a molecular-level picture that clearly separates interfacial behaviour from genuine nanoconfinement and provide guidance for predicting and controlling the structure of water in nanoscale solid-liquid environments.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"81-95"},"PeriodicalIF":3.1,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC13103939/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147757632","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Flexoelectric effect in flexible 2D nanofluidic channels. 柔性二维纳米流体通道中的柔性电效应。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d5fd00134j

Luyao Jia, Yangshi Shao, Jiabei Luo, Yuyan Su, Yujia Zhang, Xiong Pu

{"title":"Flexoelectric effect in flexible 2D nanofluidic channels.","authors":"Luyao Jia, Yangshi Shao, Jiabei Luo, Yuyan Su, Yujia Zhang, Xiong Pu","doi":"10.1039/d5fd00134j","DOIUrl":"10.1039/d5fd00134j","url":null,"abstract":"Flexoelectricity refers to the electric polarisation induced by a mechanical strain gradient. By comparison with other mechanoelectric conversion approaches, the flexoelectric effect can occur in both symmetric and asymmetric dielectric materials and exhibit pronounced effects at the nanoscale. Here, we demonstrate the generation of a flexoelectric effect in a flexible nanofluidic device comprising two-dimensional (2D) graphene oxide (GO) films. Free-standing GO films are produced to construct the aligned multilayer 2D nanofluidic channels with an angstrom-scale interlayer spacing of ∼7-12 Å. Upon bending deformation, an electrical current is detected flowing between the two electrodes attached to the GO film, showing a flexoelectric coefficient up to 188 µC m-1, which is higher than that of other reported flexoelectric devices. We combine a theoretical simulation model and experimental characterisations to demonstrate that the flexoelectric effect is generated by the cross-layer transport of hydrated ions in the multilayer GO channels. The bending deformation induces a strain gradient in the GO film, which in turn drives the movement of water and ions in the charged nanofluidic channels, generating a flexoelectric output. Our nanofluidic device may be used to build self-powered sensors and actuators in the future.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"274-288"},"PeriodicalIF":3.1,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147757780","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Operando X-ray mapping of ion transport and arrangement in a carbon-based supercapacitor electrode. 碳基超级电容器电极中离子输运和排列的操作x射线作图。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d5fd00140d

Malina Seyffertitz, Max Valentin Rauscher, Sebastian Stock, Sylvio Haas, Peter Moharitsch, Oskar Paris

{"title":"Operando X-ray mapping of ion transport and arrangement in a carbon-based supercapacitor electrode.","authors":"Malina Seyffertitz, Max Valentin Rauscher, Sebastian Stock, Sylvio Haas, Peter Moharitsch, Oskar Paris","doi":"10.1039/d5fd00140d","DOIUrl":"10.1039/d5fd00140d","url":null,"abstract":"Position- and time-resolved X-ray transmission (XRT) and small-angle X-ray scattering (SAXS) are used to map out ion transport and nanoscale ion arrangement in an in-plane carbon-based supercapacitor working electrode with 1 M RbBr aqueous electrolyte. XRT reveals that the charge balancing mechanism depends on the electrode geometry, shifting from ion exchange to predominantly Rb+ transport as the distance between working electrode and counter electrode is increased. SAXS shows that, despite these differences in ion mobilisation, the nanoscale ion arrangement within the smallest carbon nanopores remains essentially unchanged across the electrode and independent of the charging protocol. Small, but systematic differences are observed between sub-nanometre micropores (strong confinement) and larger micropores/mesopores (weaker confinement), the latter showing a distinct time dependence of ion concentration changes attributed to diffusive equilibration processes in these pores. Overall, these findings show that ion transport varies with position on the electrode, whereas the nanoscale ion arrangement does not. The smallest micropores behave uniformly across the electrode, and larger micropores and mesopores likewise show identical local arrangement at all positions, although their additional reservoir-character leads to a slight position dependent ion transport, similar to the overall bulk ion diffusion.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"44-60"},"PeriodicalIF":3.1,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147808870","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Energy-efficient time series processing in real-time with fluidic iontronic memristor circuits. 基于流体电子忆阻电路的实时高效时间序列处理。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d5fd00168d

T M Kamsma, Y Gu, C Spitoni, M Dijkstra, Y Xie, R van Roij

{"title":"Energy-efficient time series processing in real-time with fluidic iontronic memristor circuits.","authors":"T M Kamsma, Y Gu, C Spitoni, M Dijkstra, Y Xie, R van Roij","doi":"10.1039/d5fd00168d","DOIUrl":"10.1039/d5fd00168d","url":null,"abstract":"Iontronic neuromorphic computing has emerged as a rapidly expanding paradigm. The arrival of angstrom-confined iontronic devices enables ultra-low power consumption with dynamics and memory timescales that intrinsically align well with signals of natural origin, a challenging combination for conventional (solid-state) neuromorphic materials. However, comparisons to earlier conventional substrates and evaluations of concrete application domains remain a challenge for iontronics. Here we propose a pathway toward iontronic circuits that can address established time series benchmark tasks, enabling performance comparisons and highlighting possible application domains for efficient real-time time series processing. We model a Kirchhoff-governed circuit with iontronic memristors as edges, while the dynamic internal voltages serve as output vector for a linear readout function, during which energy consumption is also logged. All these aspects are integrated into the open-source pyontronics package. Without requiring input encoding or virtual timing mechanisms, our simulations demonstrate prediction performance comparable to various earlier solid-state reservoirs, notably with an exceptionally low energy consumption of over 5 orders of magnitude lower. These results suggest a pathway of iontronic technologies for ultra-low-power real-time neuromorphic computation.","PeriodicalId":76,"journal":{"name":"Faraday Discussions","volume":" ","pages":"411-427"},"PeriodicalIF":3.1,"publicationDate":"2026-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147757794","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Spiers Memorial Lecture: Breakdown of universality in angstrom-scale flows. 斯皮尔斯纪念讲座：埃尺度流中普遍性的分解。

IF 3.1 3区化学

Faraday Discussions Pub Date : 2026-09-04 DOI: 10.1039/d6fd00054a

Lydéric Bocquet

引用次数: 0