Surface charge modulation boosts electrocatalytic water splitting over iridium catalysts on a polyimide support

Zhang, Longsheng; Zhang, Shouhan; Bai, Jing; Ding, Yidan; Ye, Jinyu; Song, Yuanhao; Debroye, Elke; Fan, Wei; Liu, Tianxi

doi:10.1039/d4cc01113a

Chem. Commun.

2024

DOI: 10.1039/d4cc01113a

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Surface charge modulation boosts electrocatalytic water splitting over iridium catalysts on a polyimide support

Longsheng Zhang,

Shouhan Zhang,

Jing Bai

et al.

Abstract: Developing high-performance iridium (Ir)-based catalysts with minimal precious Ir metals is significant but challenging towards acidic oxygen evolution reaction (OER). Here, we report a high-performance OER catalyst with Ir nanoparticles...

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Cited by 3 publications

References 44 publications

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Single‐Atom Zirconium Coordination Polyimide Aerogel as Separator Coating Toward High‐Rate Lithium Metal Battery

Zhou,

Bao,

Fang

et al. 2024

Adv Funct Materials

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Developing high‐rate lithium‐metal battery (LMB) with superior energy density and operation durability is of significance, which shows enormous potential to be extensively applied. However, the commercialized polyolefin separators exhibit inferior ability to resist the elevated internal temperature and inhibit the lithium (Li) dendrite growth, especially for LMBs under high‐rate operations. With undesired Li+‐anion solvated structures in the electrolyte, previous separator modification strategies usually meet a dilemma to simultaneously increase the Li+ transference number and decrease the anion transference number. Here, a facile and scalable strategy are reported to prepare high‐performance sandwiched separators with polyolefin separators coated by single‐atom zirconium coordination polyimide aerogel (Zr‐PIA) layers, which can achieve a stable LMB operation at 20 C for 2700 cycles with a capacity retention of 94.6%, substantially outperforming its counterpart separator without Zr. Both the experimental and theoretical studies suggest that the Zr‐PIA layer with nanoporous architecture and anion‐trapping Zr sites can effectively increase the Li+ transference number without sacrificing the overall ion conductivity, enabling a rapid, selective and uniform Li+ flux through the separator. Such features can facilitate homogeneous the Li nucleation/deposition and mitigate Li dendrite growth, leading to enhanced battery durability and safety.

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Single‐Atom Zirconium Coordination Polyimide Aerogel as Separator Coating Toward High‐Rate Lithium Metal Battery

Zhou,

Bao,

Fang

et al. 2024

Adv Funct Materials

View full text Add to dashboard Cite

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Single‐Atom Platinum Immobilized on Polyimide for Highly Efficient and Durable Hydrogen Evolution Electrocatalysis

Zhang,

Wu,

Liu

et al. 2024

Advanced Energy Materials

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Electrocatalytic hydrogen evolution reaction (HER) is widely regarded as a promising approach to convert renewable electricity into hydrogen. Platinum (Pt) based catalysts demonstrate superior activity toward acidic HER, but the scarcity of Pt metal presents obstacles for large‐scale application. Therefore, constructing Pt single‐atom catalysts (SACs) with maximum metal‐atom‐utilization efficiency renders a feasible strategy, which however is critically hindered by an unsatisfactory catalyst lifetime. Here, a general strategy is reported to develop novel HER catalysts with Pt single atoms immobilized on polyimide support, which can display an exceptional activity toward acidic HER while achieving an outstandingly high durability with negligible activity decay for 760 h of continuous operation at 100 mA cm−2. The detailed experimental and theoretical results unravel that, the polyimide support lowers the d‐band level of Pt site with a reduced energy barrier for acidic HER and simultaneously promotes the proton concentration near Pt site, leading to appreciably improved HER kinetics. Additionally, the polyimide support is versatile toward immobilizing ruthenium, palladium, and other single metal atoms, providing an alternative approach to develop SACs with superior catalytic activity and durability.

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Atomically Dispersed Iridium on Polyimide Support for Acidic Oxygen Evolution

Zhang,

Bai,

Zhang

et al. 2024

ACS Nano

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Designing a high-performing iridium (Ir) single-atom catalyst is desired for acidic water electrolysis, which shows enormous potential given its high catalytic activity toward acidic oxygen evolution reaction (OER) with minimum usage of precious Ir metal. However, it still remains a substantial challenge to stabilize the Ir single atoms during the OER operation without sacrificing the activity. Here, we report a high-performing OER catalyst by immobilizing Ir single atoms on a polyimide support, which exhibits a high mass activity on a carbon paper electrode while simultaneously achieving outstanding stability with negligible decay for 360 h. The resulting electrode (denoted as Ir 1 −PI@CP) reaches a 49.7-fold improvement in mass activity compared to the counterpart electrode prepared without polyimide support. Both our experimental and theoretical results suggest that, owing to the strong metal−support interactions, the polyimide support can enhance the Ir 5d states of Ir single atoms in Ir 1 −PI@CP, which can tailor the adsorption energies of intermediates and decrease the thermodynamic barrier at the ratedetermining step of the OER, but also facilitate the proton−electron-transfer process and improve the reaction kinetics. This work offers an alternative avenue for developing single-atom catalysts with superior activity and durability toward various catalytic systems and beyond.

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Surface charge modulation boosts electrocatalytic water splitting over iridium catalysts on a polyimide support

Abstract: Developing high-performance iridium (Ir)-based catalysts with minimal precious Ir metals is significant but challenging towards acidic oxygen evolution reaction (OER). Here, we report a high-performance OER catalyst with Ir nanoparticles...

Cited by 3 publications

References 44 publications

Single‐Atom Zirconium Coordination Polyimide Aerogel as Separator Coating Toward High‐Rate Lithium Metal Battery

Single‐Atom Zirconium Coordination Polyimide Aerogel as Separator Coating Toward High‐Rate Lithium Metal Battery

Single‐Atom Platinum Immobilized on Polyimide for Highly Efficient and Durable Hydrogen Evolution Electrocatalysis

Atomically Dispersed Iridium on Polyimide Support for Acidic Oxygen Evolution

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