INORGANIC CHEMISTRY
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2025
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IF 4.7
Jun-Ru Tian,Jie-Yao Song,Zhongchang Wang
Conventional fluorescent pH sensors, despite offering high sensitivity and rapid response, are limited by their reliance on fluorescence intensity changes, hindering applications requiring precise wavelength control. Here, we present a pH sensing strategy based on cross-linked carbon quantum dots (CCL-CQDs) displaying a remarkable pH-dependent red shift in the fluorescence emission wavelength. Amino- and carboxyl-functionalized CQDs were synthesized via a one-step hydrothermal method and further assembled into CCL-CQDs through the condensation reaction between amino groups and glutaraldehyde. The CCL-CQDs displayed excellent pH sensitivity, with their fluorescence emission wavelength exhibiting a linear red shift upon increasing pH (from 2.29 to 7.16). The results of mechanism exploration revealed that H+ induced the cleavage of C═N bonds in the CCL-CQD structure, leading to the formation of –COOH groups and increased surface-oxidized carbon content. This enhanced oxidation generated more surface defects, triggering a wavelength shift in surface-state-related fluorescence emission. This study demonstrates the successful synthesis of pH-sensitive CCL-CQDs with an excellent fluorescence detection performance.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Su Yafei,Peng Huawen,Liu Xufei,Li Jiapeng,Zhao Qiang
Cation separation under extreme pH is crucial for lithium recovery from spent batteries, but conventional polyamide membranes suffer from pH-induced hydrolysis. Preparation of high performance nanofiltration membranes with excellent pH-resistance remains a challenge. Here we synthesize a high performance nanofiltration membrane (1,4,7,10-Tetraazacyclododecane (TAD)−1,3,5-Tris(bromomethyl)benzene (TBMB) thin film composite membranes (TFCMs)) with excellent pH-stability through interfacial quaternization reaction between TAD and TBMB. Due to the high stability of “C-N” bonds in TAD-TBMB TFCMs, its separation performance is stable even after 70 days immersion in concentrated acid (3 M H 2 SO 4 , HNO 3 , or HCl) and base (3 M NaOH), which is at least 15 times more stable than benchmark commercial membranes. The membrane shows an overall separation performance (11.3 L m −2 h −1 bar −1 (LMHB), R Co2+ : 97% in 2 M H 2 SO 4 ) due to the size sieving and the intensified charge repulsion, outperforming many of the state-of-the-art membranes. Finally, the TAD-TBMB TFCM remains stable during 30-days continuous nanofiltration of 2 M H 2 SO 4 and leachate (2 M H 2 SO 4 , ions: 6.2 g L −1 ) from spent batteries.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Xue Yang,Hongyi Wang,Haizhong Liu,Zhifu Yin
Additive abuse in fishery, such as tricaine methanesulfonate (MS222), ciprofloxacin (CPFX), and malachite green (MG), threatens public human health and interferes with the ecological equilibrium of water resources. However, the majority of the present detection methods suffer from high costs, complex operations, and poor portability. Therefore, real-time and rapid detection of the above additive by mobile devices is becoming increasingly important. Here we report the fabrication and performance of an entirely electrochemical system with USB-stick size for simultaneous detection of MS222, CPFX, and MG, as well as pH and permittivity. The limits of detections are 0.17, 0.67, and 0.28 µg/mL, while the resolution ratios are 10 %, 10 %, and 5 % for MS222, MG, and CPFX, respectively. For both pH and permittivity, they have linear regressions measured by brightness and capacitance of the sample respectively, at the range of 1.5–9 (pH) and 10–20 (permittivity). The interference experiments, using target analytes (40 μg/mL) and 15 interfering analytes (80 μg/mL), demonstrated the anti-interference performance of the sensor patches. The field studies on carps, catfishes, and chubs indicated that the developed integrated portable system could be used for real sample analysis with high performance.
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JOURNAL OF MEMBRANE SCIENCE
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2024
·
IF 8.4
Ning Gan,Yuqing Lin,Yiren Zhang,Yulong Qiu,Jianguo Yu,Qianhong She,Tooru Ooya,Qian Lin,Hideto Matsuyama
Tunable gating ion-conducting membranes with high water permeability and precise ion selectivity remain urgently demanded in smart nanofiltration for efficient lithium extraction . Herein, inspired by the filtration function of protein channels, we report a smart and high-performance supramolecular membrane constructed via coordination between quaternary ammonium ligands ( m -phenylenediamine/polyethyleneimine) and metal ion center (Cu 2+ ). The pore architecture of the supramolecular membrane is dynamic and can be switched by applying pH stimulus, where coordinated interchain expands when exposed to acidic operating conditions and induces concomitantly reinforced electrostatic exclusion due to enhanced local charge density. The tunable gating regularity enables operando modulation of precise ionic separation in situ. The resulting membrane exhibits significantly enhanced water permeance (19.8 L m −2 h −1 ·bar −1 ) and simultaneously promoted Li + /Mg 2+ selectivity (R Mg2+ = 96.4 %), surpassing typical trade-off between permeability and selectivity at pH 3 condition. This study demonstrates the amazing capability of environmental-responsive regulation of membrane pore-channel structure, and provides inspiration for engineering advanced supramolecular membranes for lithium extraction and beyond.
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DYES AND PIGMENTS
·
2024
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IF 4.1
Aiming Ju,Zhiguang Xu,Zhihao Huang,Tao Zhang,Yan Zhao
Humidity-induced discoloration from surface coating is promising, but the surface suffers from low stability, due to the lack of covalent interactions between pH indicator, hygroscopic components and fabrics. Here, we report a strategy to fabricate all-polymer-based, highly hygroscopic fabrics with humidity-induced discoloration and pH-induced discoloration simply by covalently coating/polymerizing a reactive pH indicator and a hygroscopic monomer onto fabrics. The resulting fabrics show remarkable and reversible discoloration from blue to yellow, upon increasing relative humidity. The high reusability of the discoloration has been verified by repeating moisture adsorption and desorption over 20 cycles, without obvious deterioration in the discoloration behavior. Moreover, the fabrics display discoloration behaviors upon contacting aqueous solutions and vapors at different pHs. The simple coating, significant and reversible color transition, and the high reusability enable the all-polymer-based, hygroscopic fabrics to be excellent candidates for humidity indication and pH indication.
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ACS Sensors
·
2024
·
IF 8.2
Zhihui Zhang,Kerui Li,Yaogang Li,Qinghong Zhang,Hongzhi Wang,Chengyi Hou
In recent years, wearable devices have been widely used for human health monitoring. Such monitoring predominantly relies on the principles of optics and electronics. However, electronic detection is susceptible to electromagnetic interference, and traditional optical fiber detection is limited in functionality and unable to simultaneously detect both physical and chemical signals. Hence, a wearable, embedded asymmetric color-blocked optical fiber sensor based on a hydrogel has been developed. Its sensing principle is grounded in the total internal reflection within the optical fiber. The method for posture sensing involves changes in the light path due to fiber bending with color blocks providing wavelength-selective modulation by absorption changes. Sweat pH sensing is facilitated by variations in fluorescence intensity triggered by sweat-induced conformational changes in Rhodamine B. With just one fiber, it achieves both physical and chemical signal detection. Fabricated using a molding technique, this fiber boasts excellent biocompatibility and can accurately discern single and multiple bending points, with a recognition range of 0–90° for a single segment, a detection limit of 0.02 mm–1 and a sweat pH sensing linear regression R2 of 0.993, alongside great light propagation properties (−0.6 dB·cm–1). With its extensive capabilities, it holds promise for applications in medical monitoring.
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Polymers
·
2024
·Vol. 16
·期 11
·1530
·
IF 4.7
Dunyi Xiao,Huiru Ma,Wei Luo,Jianguo Guan
Responsive photonic crystal hydrogel sensors are renowned for their colorimetric sensing ability and can be utilized in many fields such as medical diagnosis, environmental detection, food safety, and industrial production. Previously, our group invented responsive photonic nanochains (RPNCs), which improve the response speed of photonic crystal hydrogel sensors by at least 2 to 3 orders of magnitude. However, RPNCs are dispersed in a liquid medium, which needs a magnetic field to orient them for the generation of structural colors. In addition, during repeated use, the process of cleaning and redispersing can cause entanglement, breakage, and a loss of RPNCs, resulting in poor stability. Moreover, when mixing with the samples in liquid, the RPNCs may lead to the contamination of the samples being tested. In this paper, we incorporate one-dimensional oriented RPNCs with agarose gel film to prepare heterogeneous hydrogel films. Thanks to the non-responsive and porous nature of the agarose gel, the protons diffuse freely in the gel, which facilitates the fast response of the RPNCs. Furthermore, the “frozen” RPNCs in agarose gel not only enable the display of structural colors without the need for a magnet but also improve the cycling stability and long-term durability of the sensor, and will not contaminate the samples. This work paves the way for the application of photonic crystal sensors.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Yan Xu,Weitao Yang,Zhuoyao Wu,Hui Wang,Tianming Cui,Weiwei Zeng,Yanjing Yun,Bingbo Zhang
Effective monitoring of gastric fluid pH is crucial for diagnosing gastric diseases and evaluating anti-gastric-acid therapies. The invasiveness and low patient compliance with traditional gastric fluid aspiration methods highlight the need of a non-invasive, real-time technique for in situ gastric pH monitoring. This study introduces a novel chromium (Cr)-based magnetic resonance probe, Cr(OH) 3 @HSA, specifically designed for pH-sensitive gastric imaging. Synthesized via an albumin-mediated biomimetic mineralization process, Cr(OH) 3 @HSA possesses an amorphous structure that facilitates the sensitive release of paramagnetic Cr(III) ions in acidic environments. This release substantially decreases the longitudinal relaxation time of surrounding hydrogen protons, as demonstrated by an 18.29-fold increase in the longitudinal relaxation rate from pH 6.5 to pH 1.0. In vivo experiments show that Cr(OH) 3 @HSA accurately detects abnormal gastric pH levels and evaluates the efficacy of gastric antiacids, surpassing the performance of the conventional “always-on” contrast agent, Magnevist®. Notably, our research reveals that chromium picolinate, a common dietary supplement for diabetes, generates a “turn-on” signal in the gastrointestinal tract, suggesting potential MR signal interference in diabetic patients. Consequently, we recommend that diabetic patients avoid chromium-based dietary supplements prior to MRI procedures to prevent Cr(III)-induced signal alterations.
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Journal of Pharmaceutical Innovation
·
2024
·Vol. 19
·期 4
·1-13
·
IF 2.7
Feng Runliang,Chen Shiyu,Zhao Yingshun,Wang Mingzhu,Li Yuli,Jia Yunjing,Song Zhimei
Purpose To improve azithromycin’s antibacterial activity at different pH through combination therapy. Method Azithromycin- and ibuprofen-loaded micelles were fabricated by the self-assembly of MPEG-PVL copolymer, respectively. Results The drug-loaded micelles had controlled drug release property with water-solubility improvement. Notably, at pH 7.4 or 6.0, the in vitro antibacterial experiments demonstrated that there was no synergistic effect for the two native drugs against S. aureus , but a significant synergy was observed when the two preparations were used in combination. In vitro PI fluorescence staining experiment demonstrated that the introduction of ibuprofen-loaded micelles obviously increased cellular uptake under low concentration of azithromycin-loaded micelles. Through SEM and spectral evaluation experiments, it was found that ibuprofen-loaded micelles could increase the cell permeability by interacting with proteins and phospholipids in the cell membrane, which was conducive to promoting azithromycin-loaded micelles to enter the cells and play a drug effect. Conclusion The azithromycin- and ibuprofen-loaded micelles with synergistically enhanced antibacterial activity are potential candidates for effective bacterial combination therapy. Graphical Abstract
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ACS Nano
·
2024
·
IF 15.8
Yu Han,Jiaxiang Ma,Dongqing Liu,Yan Yang,Tao Zhang,Min Wang,Daxin Liang,Liping Wen,Jun Ma,Wei Wang
Ion-sieve adsorbents are effective materials in practical applications for extracting liquid lithium. However, it is greatly suppressed in adsorption capacity and selectivity (Li/Mg) under natural near-neutral conditions of seawater or salt lakes, due to the interference of in situ released H+ and Mg2+ impurity. This paper proposes an adsorbent with a microenvironment-modulating function as a solution. The introduction of quaternary ammonium groups into the carrier accelerates the migration of H+, while preventing the diffusion of Mg2+ by electrostatic repulsion. Besides, it can also prestore OH–, effectively consuming the generated hydrogen ions in situ. Based on the rational design, the alkali consumption of the microenvironment-modulating strategy is dramatically reduced to 1/144 of the traditional alkali-adding method. Additionally, adsorption performance is significantly promoted under natural pH conditions, with a maximum 33 times higher separation factor (selectivity) and 4 times higher adsorption capacity than commercial ion-sieve adsorbents. This development indicates the feasibility of using microenvironment modulation for effective lithium extraction and inspires the development of next-generation high-performance adsorbents.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Xiaojing Dong,Yangyang Wang,Jintao Wang,Yiqiang Sun,Bo Xu,Cuncheng Li,Lifeng Hang
In the field of research on renewable energy conversion and storage methods, the development of catalysts with excellent properties and outstanding stability for oxygen evolution reaction (OER) acting at various pH values has become a much-anticipated research focus. RuO 2 as a benchmark OER catalyst, its wide application has always been limited by slow reaction kinetics and limited persistence. In this paper, Mn-doped RuO 2 material was developed and the optimum doping ratio was identified for using as an OER electrocatalyst under general purpose pH media. Mn 0.1 Ru 0.9 O 2 exhibited a lower overpotential value of 224 mV in acidic environment with a Tafel slope value of 51.62 mV dec −1 . Moreover, in alkaline and neutral environments, overpotentials of 231 mV and 376 mV were required to obtain a current density of 10 mA cm −2 , respectively. In addition, through continuous stability testing over 24 h in alkaline, acidic and neutral solutions, it has been further demonstrated that the Mn-doped RuO 2 material exhibits extremely high stability. The advancements in this research offer crucial insight into the rational development of efficient and durable RuO 2 -based catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Ranran Wei,Xiaoying Zhang,Min Yan,Xianlong Wang,Xuewen Wei,Runqi Zhang,Yinglong Wang,Liang Wang,Shuli Yin
Compared with layered materials such as graphite and transition metal disulfide compounds with highly anisotropic in-plane covalent bonds , it is inherently more challenging to obtain independent metallic two-dimensional films with atomic thickness. In this study, PtNi layered metallene nanobowls (LMBs) with multilayer atomic-scale nanosheets and bowl-like structures have been synthesized in one step using structural and electronic effects. The material has the advantage of catalyzing pH-universal hydrogen evolution reaction (HER). Compared with Pt/C, PtNi LMBs exhibited excellent HER activity and stability under all pH conditions. The overpotentials of 10 mA cm −2 at 0.5 M H 2 SO 4 , 1.0 M phosphate buffer and 1.0 M KOH were 14.8, 20.3, and 34.0 mV, respectively. Under acidic, neutral and alkaline conditions, the HER Faraday efficiencies reach 98.97%, 98.85%, and 99.04%, respectively. This study provides an example for the preparation of unique multilayer nanobowls, and also provides a basic research platform for the development of special HER materials.
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