arXiv subjects

Jianhao Qian

Publications and source records attributed to Jianhao Qian.

3 recordsLinked to original sources

arXiv2026

Competing Energetics Govern Gas Permeation in Polymer of Intrinsic Microporosity (PIM) Membranes

Polymer membranes, particularly polymers of intrinsic microporosity (PIMs), hold great promise for gas separation applications. However, the long-dominant solution-diffusion model, which treats the membrane as a nonporous homogeneous medium, does not resolve how gas-solid atomic interactions govern molecular transport in intrinsic micropores, limiting rational bottom-up membrane design. In this work, we employ non-equilibrium molecular dynamics simulations to investigate the permeation of various gases (He, H2, CH4, N2, O2, and CO2) through PIM-1 as a representative PIM membrane across a range of temperatures. By analyzing the scaling of gas permeability with molecular mass, we identify a temperature-induced transition in the dominant transport mechanism. We demonstrate that this transition is governed by the competition between gas-wall interaction potential energy and thermal kinetic energy: weak interactions or elevated temperatures facilitate Knudsen-type ballistic transport, whereas strong interactions and lower temperatures favor adsorption-mediated surface diffusion. Furthermore, molecular trajectory analysis at the membrane interface reveals two distinct entry pathways: direct entry through pore openings and surface-diffusion-assisted entry. The surface-diffusion-assisted pathway greatly promotes the entry of strongly interacting gases into the membrane, contributing to higher overall permeability, albeit this enhancement diminishes with increasing temperature. These findings offer a mechanistic picture of gas permeation in PIM-1 and explain the dependence of gas permeation on both gas type and temperature. More broadly, they highlight the importance of adopting a pore-flow perspective to understand gas transport in microporous polymer membranes.

physics.chem-ph↗

arXiv2025

Tuneable ion selectivity in vermiculite membranes intercalated with unexchangeable ions

Membranes selective to ions of the same charge are increasingly sought for wastewater processing and valuable element recovery. However, while narrow channels are known to be essential, other membrane parameters remain difficult to identify and control. Here we show that Zr$^{4+}$, Sn$^{4+}$, Ir$^{4+}$, and La$^{3+}$ ions intercalated into vermiculite laminate membranes become effectively unexchangeable, creating stable channels, one to two water layers wide, that exhibit robust and tuneable ion selectivity. Ion permeability in these membranes spans five orders of magnitude, following a trend dictated by the ions' Gibbs free energy of hydration. Unexpectedly, different intercalated ions lead to two distinct monovalent ion selectivity sequences, despite producing channels of identical width. The selectivity instead correlates with the membranes' stiffness and the entropy of hydration of the intercalated ions. These results introduce a new ion selectivity mechanism driven by entropic and mechanical effects, beyond classical size and charge exclusion.

cond-mat.soft↗

arXiv2020

DC electricity generation from dynamic polarized water-semiconductor interface

Liquid electricity generator and hydrovoltaic technology have received numerous attentions, which can be divided into horizontal movement generator and vertical movement generator. The horizontal movement generator is limited for powering the integrated and miniaturized energy chip as the current output direction is depending on the moving direction of the water droplet, which means a sustainable and continuous direct-current (DC) electricity output can be hardly achieved because of the film of limited length. On the other hand, the existing vertical movement generators include triboelectricity or humidity gradient-based liquid electricity generator, where the liquid or water resource must be sustainably supplied to ensure continuous current output. Herein, we have designed an integratable vertical generator by sandwiching water droplets with semiconductor and metal, such as graphene or aluminum. This generator, named as polarized liquid molecular generator (PLMG), directly converts the lateral kinetic energy of water droplet into vertical DC electricity with an output voltage of up to ~1.0 V from the dynamic water-semiconductor interface. The fundamental discovery of PLMG is related to the non-symmetric structure of liquid molecules, such as water and alcohols, which can be polarized under the guidance of built-in field caused by the Fermi level difference between metal and semiconductor, while the symmetric liquid molecules cannot produce any electricity on the opposite. Integratable PLMG with a large output power of ~90 nW and voltage of ~2.7 V has been demonstrated, meanwhile its small internal resistance of ~250 kilohm takes a huge advantage in resistance matching with the impedance of electron components. The PLMG shows potential application value in the Internet of Things (IoTs) after proper miniaturization and integration.

physics.app-ph↗