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Journal of Materials Chemistry C · 2023 ·Vol. 11 ·期 5 ·1960-1970 · IF 6.4

Color-tunable and ultralong organic room temperature phosphorescence from poly(acrylic acid)-based materials through hydrogen bond engineering

Liuqi Kong,Yan Zhu,Shaochen Sun,Hongye Li,Farong Tao,Fei Li,Liping Wang,Guang Li

Color-tunable and ultralong organic room temperature phosphorescence (URTP) materials have drawn extensive attention due to their various applications in many fields. Herein, a series of poly(acrylic acid) (PAA)-based RTP materials are facilely constructed through hydrogen bond engineering by binary doping of PAA with phenylboric acid and benzoic acid derivatives. PAA-based RTP materials all exhibit long lifetimes, and PAA–4-carboxyphenylboronic acid (PAA–CPBA) shows durable afterglow (more than 12 s) with an ultralong phosphorescence lifetime (up to 536 ms) under ambient conditions. PAA–1,4-benzendiboronic acid (PAA–BDA) displays multicolor tunable phosphorescence by changing the excitation wavelengths or BDA doping concentrations. Most impressively, the phosphorescence color of PAA–CPBA can change from blue to green by water vapor fumigation, and return to blue again through heating treatment. After sequential water vapor and heating treatment, the phosphorescence peak of PAA–CPBA is red-shifted from 425 nm to 525 nm with the excitation wavelength increasing from 230 to 300 nm. PAA-based RTP materials are further applied in information encryption and rewritable paper on the basis of the properties of ultralong luminescence lifetime and color-tunability. This work provides inspiration for the design and preparation of color-tunable polymer-based URTP materials.

CAS / MDL: 98-80-6 78-67-1
研究领域: 材料科学 · 光学
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Science Advances · 2024 ·Vol. 10 ·期 40 · IF 11.7

In situ continuous hydrogen-bonded engineering for intrinsically stretchable and healable high-mobility polymer semiconductors

Haoguo Yue,Ying Wang,Shaochuan Luo,Junfeng Guo,Jun Jin,Gongxi Li,Zhihao Meng,Lei Zhang,Dongshan Zhou,Yonggang Zhen,Wenping Hu

As a key component for wearable electronics, intrinsically stretchable and healable semiconducting polymers are scarce because carrier mobility is often reduced with increasing stretchability and self-healability. Here, we combine stepwise polymerization and thermal conversion to introduce in situ continuous hydrogen bonding sites in a polymer backbone without breaking the conjugation or introducing bulky softer side chains, benefiting the intrachain and interchain charge transport. We demonstrate that a regular sequence structure facilitated the formation of big nanofibers with a high degree of aggregation, providing the loose and porous thin film with simultaneously improved charge transport, stretchability, and self-healability. The mobility of damaged devices can be recovered to 81% after a healing treatment. Fully stretchable transistor based on the designed polymer exhibited a greatly enhanced mobility up to 1.08 square centimeters per volt per second under 100% strain, which is an unprecedented value and constitutes a major step for the development of intrinsically stretchable and healable semiconducting polymers.

研究领域: 材料科学 · 有机电子学 · 柔性电子
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Gallate-based metal–organic frameworks for the selective removal of trace ammonia via hydrogen bond engineering

Peng Wu,Zai-Dong Shao,George Z. Chen,Jun He,Yu-Ming Zheng

Ammonia (NH 3 ) is a prevalent indoor pollutant, particularly in semiconductor cleanrooms, where it is essential to adhere to stringent regulations that maintain concentration levels below parts per million (ppm). The development of sustainable adsorbents exhibiting high selectivity and adsorption capacity for NH 3 at low partial pressures constitutes a critical yet challenging endeavor within this field. Herein, we introduce a class of isostructural gallate-based metal–organic frameworks (M−GA MOFs, M = Co, Mg, and Mn) endowed with abundant hydrogen bond donors within the pore channels. Notably, the Co-GA MOF exhibits an exceptionally high NH 3 uptake of 3 mmol g −1 at an ultralow pressure of 0.001 mbar, surpassing all previously reported MOFs. Density-functional theory (DFT), independent gradient model based on Hirshfeld partition (IGMH), and quantum theory of atoms in molecules (QTAIM) analyses reveal the presence of strong O-H···N and N-H···O hydrogen bonds between NH 3 and the MOF framework. These interactions, combined with van der Waals forces, contributed to exceptional NH 3 selectivity over CO 2 and N 2 , with selectivity exceeding 10 4 for NH 3 /CO 2  = 0.1 %:99.9 %. Breakthrough experiments validate the exceptional removal performance of Co-GA MOFs for trace amounts of NH 3 , with a breakthrough point observed at 14 d g −1 for a concentration of 10 ppm NH 3 . This work not only advances our understanding of ultralow-pressure gas separation mechanisms but also offers a scalable solution for efficient separation and purification of trace contaminants in environmentally relevant settings.

CAS / MDL: 5995-86-8
研究领域: 材料科学 · 环境科学 · 化学工程
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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 33 ·期 3 ·2210395 · IF 19.924

Strong and Ultra-Tough Supramolecular Hydrogel Enabled by Strain-Induced Microphase Separation

Jiayu Wu,Zhixing Zhang,Zhenyuan Wu,Desheng Liu,Xingxing Yang,Yixian Wang,Xin Jia,Xin Xu,Pan Jiang,Xiaolong Wang

Architected hydrogels are widely used in biomedicine, soft robots, and flexible electronics while still possess big challenges in strong toughness, and shape modeling. Here, inspired with the universal hydrogen bonding interactions in biological systems, a strain-induced microphase separation path toward achieving the printable, tough supramolecular polymer hydrogels by hydrogen bond engineering is developed. Specifically, it subtly designs and fabricates the poly (N-acryloylsemicarbazide-co-acrylic acid) hydrogels with high hydrogen bond energy by phase conversion induced hydrogen bond reconstruction. The resultant hydrogels exhibited the unique strain-induced microphase separation behavior, resulting in the excellent strong toughness with, for example, an ultimate stress of 9.1 ± 0.3 MPa, strain levels of 1020 ± 126%, toughness of 33.7 ± 6.6 MJ m −3 , and fracture energy of 171.1 ± 34.3 kJ m −2 . More importantly, the hydrogen bond engineered supramolecular hydrogels possess dynamic shape memory character, i.e shape fixing at low temperature while recovery after heating. As the proof of concept, the tailored hydrogel stents are readily manufactured by 3D printing, which showed good biocompatibility, load-bearing and drug elution, being beneficial for the biomedical applications. It is believed that the present 3D printing of the architected dynamic hydrogels with ultrahigh toughness can broaden their applications.

研究领域: 生物医学 · 材料科学 · 软体机器人 · 柔性电子
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Journal of Materials Chemistry C · 2025 · IF 5.1

A damping hydrogel with high water retention and strong adhesion for precise bioelectric signals detection

Chengyi Hou,Hongzhi Wang,Siyu Lu,Qinghong Zhang,Kerui Li,Yaogang Li,Lingli Qu,Jiabei Luo

Bioelectric signals are important for understanding biological patterns and treating diseases. However, the detection of bioelectric signals is often interfered by the artifacts caused by unintentional human movements, therefore, the damping of the interface experiencing vibrations is crucial for obtaining clear bioelectric signals. Herein, we propose a hydrogen bond-engineered dual-network hydrogel damper via photopolymerization strategy, incorporating acetamide (AC) molecules as dynamic bonding regulators. The amphiphilic nature of AC can act as both a hydrogen bond donor and acceptor, contributing to the construction of a high-density interpenetrating hydrogen bond network in chitosan/acrylic matrices. The hydrogel damper exhibits high water retention (8% water loss for 5 days at 25 ℃, 54% RH), strong adhesion (93.42 kPa on skin), and high damping performance (tan δ > 0.3) in the human movement frequency range (1-50 Hz). Due to these properties, the hydrogel is firmly attached to the human skin, reducing the interface impedance between the hydrogel damper and the skin, and can be stored at room temperature for a long time without losing water. In addition, the hydrogel damper has a frequency-dependent dynamic mechanical behaviour that selectively removes motion artifacts to improve the stability and reliability of the bioelectric signal acquisition.

CAS / MDL: 7473-98-5
研究领域: 生物医学工程 · 材料科学
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2025 · IF 1.6

Extraction of uranium with Hydrogen-Bonded Complex Extractants based on TBPO: chemical structure, performance and mechanism

Tao Qinqin,Wang Yusheng,Chen Chuanhong,Dai Ying

This study investigates the role of hydrogen bonding in Hydrogen-Bonded Complex Extractants (HBCEs) for uranium extraction from wastewater. Through integrated experimental and theoretical approaches including electrostatic potential (ESP) analysis, molecular binding energy calculations, Atoms in Molecules (AIM) theory, and spectroscopic characterization, we reveal how structural variations (carbon chain length, unsaturation degree, spatial configuration, and functional groups) modulate hydrogen bond characteristics. Results show that extending carbon chains enhances hydrogen bond strength (TBPO-18: -24.28 kcal/mol binding energy), while increasing unsaturation initially weakens then strengthens interactions. Linear structures exhibit superior hydrogen bonding versus cyclic configurations (TBPO-OH vs TBPO-HOH: 18.60 vs 14.47 kcal/mol). Extraction performance correlates with hydrogen bond stability, where TBPO-12 achieves maximum capacity (40.55 mg/L) due to optimal acid resistance. Mechanistic studies via 31 P NMR titration confirm a two-step process: initial \({\text{UO}}_{2}^{2 + }\) complexation with TBPO’s P = O group, followed by hydrogen bond formation with HBDs. This work provides fundamental insights for rational design of high-efficiency HBCEs, highlighting hydrogen bond engineering as a key strategy for nuclear wastewater treatment.

研究领域: 核化学 · 环境科学 · 分离技术 · 材料科学 · 物理化学
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Materials Today Chemistry · 2025 · IF 6.7

The birefringence optimization by hydroxyl in organic nonlinear optical crystals

Lilin Yang,Hanxiang Mi,Qinghe Li,Dongling Yang,Hongyuan Sha,Zujian Wang,Rongbing Su,Bin Su,Chao He

Owing to the urgent requirement of short-wave ultraviolet (UV) nonlinear optical (NLO) crystals, organics with planar groups attract much attention, which usually exhibit a high optical anisotropy and a large second harmonic generation (SHG) response. Herein, we found glycolamide crystals based on the structure modulation of acetamide by hydroxyl. With a staggered arrangement of planar groups, acetamide crystal exhibits such an insufficient optical anisotropy that could not satisfy the phase-matching condition. To address this limitation, a targeted molecular engineering approach was implemented by introducing hydroxyl into methyl, which induces a configuration reconstruction by dual hydrogen bonds, resulting in a uniformly arranged glycolamide structure. As a bifunctional unit (acting as both a hydrogen donor and an acceptor), the hydroxyl improves not only the uniformity of molecular arrangement, but also their spatial density. Therefore, glycolamide crystals exhibit a substantially modified birefringence (0.07 @ 546 nm) and an enhanced SHG response (1.6 × KH 2 PO 4 ), while they maintain a short UV absorption cutoff edge (about 210 nm). This work establishes a novel paradigm for performance optimization in organic NLO crystals by rational hydrogen bond engineering.

CAS / MDL: 598-42-5 60-35-5
研究领域: 材料科学 · 光学工程 · 凝聚态物理 · 分子晶体工程 · 非线性光学
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Journal of Energy Storage · 2025 · IF 9.8

Hydrogen-bond engineering of polyethylene glycol/aramid nanofiber separators via phase transition for high-safety and high-energy lithium-sulfur batteries

Guanhao Qi,Jiahao Ma,Chengye Mao,Yanan Sun,Zhenli Li,Yang Hao,Shanshan Gao,Xiaoming Song,Fushan Chen

High performance and safety are essential prerequisites for the large-scale application of future energy storage systems. Lithium-sulfur (Li-S) batteries have garnered significant attention from the scientific community due to their high energy density and cost-effectiveness. However, challenges such as the polysulfide shuttle effect, thermal instability of commercial separators, and insufficient mechanical strength continue to hinder the commercialization of Li-S batteries. This paper presents a fabrication process for a hydrogen-bond-based polyethylene glycol (PEG)-modified aramid nanofiber (ANF) composite separator (PEG/ANF separator). The inherent properties of aramid nanofibers combined with PEG's unique flexible ether chain structure endow this separator with exceptional thermal stability (no dimensional shrinkage even at 200 °C), while also suppressing polysulfide shuttle effects and lithium dendrite growth. Results demonstrate that the PEG/ANFs separator exhibits an initial discharge specific capacity of up to 876.6 mAh·g −1 and maintains an average coulombic efficiency of 99.575 % after 300 cycles at 0.1C. This approach provides a scalable solution for designing highly safe and reliable energy storage devices.

CAS / MDL: 872-50-4
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