Science China-Chemistry
·
2014
·Vol. 57
·期 5
·662-668
·
IF 1.516
Chai YunFeng,Pan YuanJiang
Protonation and alkali-metal cation adduction are the most important ionization processes in soft-ionization mass spectrometry. Studies on the fragmentation mechanism of protonated and alkali-metal-cationized compounds in tandem mass spectrometry are essential and helpful for structural analysis. In some cases, it was often observed that a compound attached by different alkali-metal cations (or proton) exhibits similar fragmentation patterns but the relative abundances of product ions are different. This difference was considered to derive from the different electrostatic interactions of alkali-metal cations (or the bonded effect of proton) with the analyte. The alkali-metal cation with a smaller ionic radius shows stronger electrostatic interaction with the molecule because of its higher charge density. In addition, the bonded effect of the proton is stronger than the electrostatic interaction of the alkali-metal cation. In the present study, which used McLafferty-type rearrangements of even-electron ions ([M + Cat] + , Cat = H, Li, Na, K) as model reactions, the effect of cation size in mass spectrometric fragmentation reactions is highlighted. These considerations were also successfully applied to interpret the similar but distinct fragmentation behavior of proton and alkali-metal cation adducts of a synthetic compound (2-(acetamido(phenyl)methyl)-3-oxobutanoate) and a drug (entecavir).
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Haijun Chen,Chunli Kang,Shiyi Zhao,Zhuowen Wang,Haiyang Liu,Deming Dong,Jiao Qu,Na Zheng,Xiuyi Hua
Ineffective separation of photo-carriers and slow photoreaction rates seriously limit the decontamination effectiveness of the photocatalyst. To overcome these limitations, herein, the oxygen vacancies modified Z-scheme Ag 3 PO 4 /FeSnO(OH) 5 heterojunction was designed with FeSnO(OH) 5 as a co-catalyst. In this photosystem, Ag 3 PO 4 and FeSnO(OH) 5 function as oxidation and reduction centers of Ag 3 PO 4 /FeSnO(OH) 5 photocatalysts, respectively. Importantly, oxygen vacancies in the Z-scheme heterojunction provide an effective charge transport pathway, which not only inhibits the photocorrosion of Ag 3 PO 4 but also reduces electron-hole recombination, significantly boosting the photocatalytic decontamination performance and long-term stability of the Ag 3 PO 4 /FeSnO(OH) 5 photocatalyst. Remarkably, the Ag 3 PO 4 /FeSnO(OH) 5 photocatalyst demonstrated outstanding photocatalytic performance, 100 % degrading indomethacin (IDM) under visible light in just 30 min through the main generation of h + that attacks the active atoms of IDM, prominently outperforming other counterparts. Besides, three principal degradation pathways were proposed, and the toxicity of the degradation products was significantly reduced. The Ag 3 PO 4 /FeSnO(OH) 5 exhibited high photocatalytic degradation efficacy across different qualities of water. This research offers an oxygen vacancy modified engineering combined with a Z-scheme heterojunction strategy for constructing extraordinary photocatalysts for environmental purification.
✓ 已验证
DOI
高影响因子
RARE METALS
·
2025
·
IF 11
Xiaolei Wu,Ren Huang,Yibing Zhang,Peng Lv,Suhua Chen,Ying Bai
en The polyanionic compound Na 3 V 2 (PO 4 ) 3 (NVP) has emerged as a competitive cathode material for sodium-ion batteries (SIBs), owing to its high-voltage redox activity (3.4 V vs. the Na + /Na reference couple) and NASICON-type framework that enables superior ionic conductivity. However, the electrochemical performance of NVP is hampered by low intrinsic electronic conductivity, particularly under ultra-fast charging and long-term cycling conditions. Herein, a hierarchical micro-nano flower-like Na 3 V 2 (PO 4 ) 3 with a carbon-coating layer (HF-NVP@C) is synthesized by a facile n-propanol-assisted precipitation method. Theoretical analysis and experimental tests reveal that the polar-driven hydrogen bond engineering, manifested in the distinct molecular interaction between n-propanol and ultrapure water (characterized by a shorter O-H bond length of 1.859 Å and higher binding energy of −0.312 eV compared to methanol and ethanol counterparts), underpins the formation of the unique hierarchical micro-nano flower-like architecture. This hierarchical architecture creates an expanded interfacial area, enhances ionic transport pathways, and increases electrochemically active sites. Furthermore, a glucose-derived carbon coating (∼2 nm in thickness) uniformly adheres to the NVP surface, effectively enhancing its electronic conductivity. Thus, the constructed HF-NVP@C exhibits superior rate capability (68.1 mAh g −1 at 150C) and long-term cycling stability (58.7% capacity retention after 5000 cycles at 1C). This work proposes a viable strategy for designing high-performance polyanionic cathodes using hydrogen bond engineering. 摘要 zh 聚阴离子化合物Na 3 V 2 (PO 4 ) 3 @C(NVP)因其具有高电压氧化还原活性(相对于Na + /Na参比电对为3.4 V)以及能实现优异离子电导率的NASICON型骨架结构,已成为一种具有竞争力的钠离子电池(SIBs)正极材料。然而,由于NVP的本征电子电导率较低,导致其在超快充电和长期循环条件下的电化学性能较差。在本文中,通过一种简便的正丙醇辅助沉淀法合成了具有碳包覆层的分级微-纳花状Na 3 V 2 (PO 4 ) 3 @C(HF-NVP@C)。理论分析和实验测试表明,极性驱动的氢键工程体现在正丙醇与超纯水之间独特的分子相互作用上(其O-H键长为1.859 Å,比甲醇和乙醇对应的键长更短,结合能更高-0.312 eV),是形成这种独特分级微-纳花状结构的基础。这种分级结构扩大了活性材料的面积,增强其离子传输通道,并增加电化学活性位点。此外,葡萄糖衍生的碳涂层(约2 nm厚)均匀地附着在NVP表面,有效提高其电子电导率。因此,构建的HF-NVP@C展现出优异的倍率性能(150C下为68.1 mAh g -1 )和长期循环稳定性(1C下循环5000次后容量保持率为58.7%)。这项工作证明氢键工程设计高性能聚阴离子正极材料策略的可行,同时也为开发高性能钠离子电池正极材料提供了研究基础。
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2013
·Vol. 1
·期 16
·5031-5036
·
IF 0
Chu Liang,Yongfeng Liu,Mingxia Gao,Hongge Pan
In this paper, we report a KOH-doped Mg(NH2)2–2LiH system with low operating temperatures and good cycling stability. The Mg(NH2)2–2LiH–0.07KOH sample can reversibly desorb/absorb ∼4.92 wt% hydrogen with a starting and peak dehydrogenation temperature of ∼75 °C and ∼120 °C, respectively, the lowest in the current Mg(NH2)2–2LiH system studied. Moreover, the cycling stability of de-/hydrogenation is also remarkably improved by KOH doping as the average capacity degradation of the Mg(NH2)2–2LiH–0.07KOH system is of only 0.002 wt% per cycle within 30 cycles. Detailed structural investigations reveal that during ball milling, the doped KOH can react with Mg(NH2)2 and LiH to convert to MgO, KH and Li2K(NH2)3, which work together to provide the synergistic effects of thermodynamics and kinetics on hydrogen desorption and absorption of the Mg(NH2)2–2LiH system upon heating, consequently inducing a significant improvement in hydrogen storage properties.
✓ 已验证
DOI
MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
·
IF 4.182
Weina Shi,Yanqing Zhu,Cong Shen,Jifu Shi,Gang Xu,Xiudi Xiao,Runqiang Cao
Thermochemical heat storage based on inorganic salt hydrates is a promising approach to relieve the heat energy supply and demand conflicts, but there exist lots of defects of pure salts when applied to the thermochemical. This paper attempted to use functionalized Metal-Organic Frameworks (MOFs) as the porous matrices to improve the heat storage performance of inorganic salt hydrates. A series of MOFs/CaCl 2 composites based on MIL-101(Cr)-X (X = -NH 2 , –SO 3 H, H, –CH 3 , –F) were successfully synthesized and fully characterized by combining multiple techniques (i.e. powder X-ray diffraction, scanning electron microscopy , energy-dispersive X-ray analysis, N 2 adsorption-desorption, Fourier transform infrared spectroscopy , thermogravimetric and differential scanning calorimetry). The water sorption properties of the series of MOFs/CaCl 2 composites were studied during the hydration process, and a continuous adsorption/desorption experiment was also performed to investigate the cycle stability of the MOFs/CaCl 2 composites. The results show that the hydrophilic MOFs based composites have higher water sorption capacity (0.6 g(H 2 O)/g(sample) for MIL-101(Cr)–SO 3 H/CaCl 2 ) accompanied with higher heat storage density (1274 J/g for MIL-101(Cr)–SO 3 H/CaCl 2 ). Moreover, the series of MOFs all presented excellent cycle performance with little loss after continuous 17 adsorption/desorption cycles.
✓ 已验证
DOI
高影响因子
MATERIALS AND STRUCTURES
·
2026
·Vol. 59
·期 6
·303
·
IF 3.9
Yin Jianhao,Liao Jiaxin,Kong Xiangming
The composition, moisture distribution, and microstructural evolutions of calcium-silicate-hydrate (C–S–H) in synthetic C–S–H (SynCSH) and hardened tricalcium silicate paste (HC 3 SP) during the first drying-resaturation (D-R) cycle were systematically compared using low-field 1 H-nuclear magnetic resonance (LF-NMR) and thermogravimetric analysis (TGA). The stoichiometric formulas of C–S–H in SynCSH and HC 3 SP were determined as C 0.9 SH 3.65 and C 2.0 SH 4.53 , respectively. Water contents of C–S–H quantified by TGA and LF-NMR exhibit good linear relationship. Three types of water, interlayer water, gel water and capillary water in C–S–H were identified by LF-NMR. Notable observations included the abnormal increase of interlayer water during the drying process and subsequent decrease during resaturation, along with irreversible decreases in capillary water and increases in gel water after D-R cycle, which were attributed to the rearrangement of C–S–H layered structures. SynCSH exhibited collapse of capillary pore structures following the D-R cycle, resulting in irreversible reductions in total water content. This finding confirms the validity of synthetic C–S–H as a model material for cementitious C–S–H research while highlighting its limitations in predicting the microstructural stability of real cement pastes under moisture cycling.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Youheng Yao,Gaoxu Han,Yixuan Yao,Chuanjin Wang,Junshu Wu,Wenyuan Zhou,Yongli Li,Jinshu Wang
A TiCl 3 -based route enables H insertion and dispersed Ti sites on WO 3 photoanode. • Dispersed Ti sites favor secondary-hydroxyl activation and DHA formation. • H insertion suppresses free •OH species and mitigates DHA overoxidation. • (H,Ti)/WO 3 achieves 71.9% DHA selectivity and 264.5 mmol m −2 h −1 productivity. Selective photoelectrochemical oxidation of glycerol to dihydroxyacetone (DHA) offers a compelling strategy for integrating solar energy conversion with biomass valorization. However, efficient DHA accumulation remains challenging because two key issues are often underemphasized: the atomic level control of glycerol adsorption geometry for secondary-hydroxyl oxidation, and the suppression of radical mediated overoxidation of the formed DHA. Herein, we report a H, Ti-dual-modified WO 3 photoanode (H,Ti)/WO 3 that enables highly selective glycerol oxidation to DHA via cooperative interfacial pathway regulation. The (H,Ti)/WO 3 photoanode achieves a DHA selectivity of 71.9%—a sharp rise from 35.7% for WO 3 , and a DHA production rate of 264.5 mmol m −2 h −1 , roughly 5 times that of the unmodified counterpart. Mechanistically, highly dispersed Ti sites enhance adsorption of the secondary hydroxyl group of glycerol, directing the pathway toward DHA via two‑electron transfer. H‑insertion, in contrast, shifting hydroxyl chemistry away from free •OH mediated deep oxidation toward more surface-bound hydroxyl species and thereby suppressing DHA overoxidation. With this dual-pronged strategy, our work provides new insights into the selective formation and stable accumulation of DHA in biomass photoelectrochemical systems. Download: Download high-res image (146KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
POLYMER
·
2026
·
IF 5.1
Shuai Huang,Ziqiang Xiang,Yuhao Zhu,Renfeng Gong,Yicheng Wang,Ruoyi Liu,Guanjun Liu,Qingshan Wu
The rapid evolution of high-power flexible electronics necessitates materials that concurrently enable efficient heat dissipation and high-precision thermal monitoring. Conventional ionogels suffer from intrinsically low thermal conductivity, which induces severe thermal hysteresis, fundamentally compromising their accuracy in dynamic thermal detection. Herein, rather than treating copolymer regulation or h-BN filling as isolated design elements, we propose a thermally coupled ionogel design aimed at reconciling two usually conflicting requirements: rapid heat equilibration and high thermoresistive sensitivity. P(DMAA-co-AAM)/h-BN composite ionogels are fabricated via in-situ UV-initiated free-radical polymerization, in which N,N-dimethylacrylamide (DMAA) and acrylamide (AAM) form a mechanically compliant and ion-transportable copolymer network, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) provides thermally activated ionic pathways, and hexagonal boron nitride (h-BN) nanosheets introduce filler-assisted thermal transport pathways. Systematic optimization reveals that a DMAA-to-AAM mass ratio of 3:1 with 20 wt% h-BN yields the optimal synergy among mechanical flexibility, thermal transport, and ionic conduction. The resulting composite achieves a thermal conductivity of 0.469 W/(m·K), representing a ∼160% enhancement over the pristine matrix, which effectively suppresses heat accumulation. Concurrently, the ionogel exhibits an ultra-high temperature coefficient of resistance (TCR) of −13.5%/°C and a thermosensitive coefficient (B value) of 3879 K within 0-20°C. Benefiting from the enhanced thermal transport performance, the dynamic thermal response speed of this series of ionogel sensors (30°C → 35°C) is significantly accelerated with the increase of h-BN loading: the T90 response time of the 10 wt%, 20 wt%, and 30 wt% h-BN samples is 32.40 s, 24.34 s, and 15.14 s respectively. Meanwhile, the devices can still maintain stable and reversible resistance switching characteristics over 50 heating-cooling cycles. This study achieves the synergistic enhancement of the thermal management and temperature sensing performance of the ionogel, providing an ideal material platform for the next-generation wearable electronic devices and intelligent thermal management systems.
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2026
·
IF 9.2
Jian Ma,Jinfeng Sun,Liang Tian,Xiaoyu Bai,Zhuqing Yu
The recycling of waste cathode ray tube (CRT) glass in cement-based materials is hindered by its low early age reactivity which limits mechanical performance and large-scale utilization. This study presents a novel strategy to overcome this limitation by incorporating C-S-H seedings into waste CRT glass-Portland cement (PC) systems. Through a multi scale investigation encompassing workability compressive strength hydration kinetics phase assemblage and pore structure we demonstrate that C-S-H seedings act as both nucleation sites and physical fillers significantly accelerating early age hydration and promoting later pozzolanic reactions. An optimal seeding content of 1.5 wt enhanced 1 d compressive strength by 50.0% compared to the control and even surpassed pure PC by 40.5%. Notably total porosity was reduced by up to 63.2% at 1 d and the critical pore diameter was substantially refined. These improvements are attributed to a dual stage mechanism involving early age nucleation seeding and pore filling followed by enhanced pozzolanic reaction of waste glass at later ages. This work provides a scalable and effective approach for valorizing waste CRT glass in sustainable cementitious materials with a carbon emission reduction of 11.17% compared to conventional PC. The findings also highlight the need for future research on long term durability and life cycle assessment to support practical deployment.
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Shaoxia Guo,Mengting Li,Liang Gao,Yongrui Wang,Cheng Gu,Longxiao Yang,Yuping Huang,Enhui Xing,Yibin Luo,Xinbin Ma,Xingtian Shu
A series of heterogeneous Pd-catalysts was prepared via a facile new method. • Use of zeolite on EMC in C 2 mixture greatly reduced the corrosiveness of system. • The H-Beta zeolite catalyst with SiO 2 /Al 2 O 3 ratio of 22 showed superior performance. • The cooperation of H-Beta and trace MSA in presence of H 2 O boosted C 2 H 4 conversion. • A possible reaction mechanism was proposed for heterogeneous Pd-based system. Ethylene methoxycarbonylation (EMC) is highly efficient route for converting ethylene to methyl propionate (MP) with 100% atom economy, which has been commercialized over homogeneous Pd-based catalyst in pure ethylene. However, concerns about severe corrosiveness of strong liquid acids have always existed. Herein, H-Beta zeolite for the first time was introduced to cooperate with trace methanesulfonic acid (MSA) in the presence of water, to catalyze EMC in C 2 mixture. Over WMB-22 catalyst (containing H-Beta zeolite with SiO 2 /Al 2 O 3 ratio of 22, 0.32 wt% H 2 O, 0.005 wt% MSA, palladium/1,2-bis(di- tert -butylphosphinomethyl) benzene (d t bpx) complex with Pd/d t bpx/MSA ratio of 1/2/0.5), a superior ethylene conversion of 97.9% and 100% product selectivity, were obtained with C 2 H 6 /C 2 H 4 /CO feeding ratio of 1/2/2. A good linear correlation between C 2 H 4 conversions and the total acid content of H-Beta zeolite and MSA revealed that the synergistic effect between H-Beta zeolite and MSA could enhance C 2 H 4 conversion. Compared with the homogeneous catalyst with Pd/d t bpx/MSA of 1/2/15, under similar C 2 H 4 conversion conditions, the MSA amount of heterogeneous system was 1/30 of homogeneous system, indicating the addition of zeolite could greatly reduce the corrosiveness of system. 31 P nuclear magnetic resonance (NMR) results indicated that the introduction of zeolite, water and MSA could promote the generation and stabilization of active species. 1 H magic angle spinning (MAS) NMR and isotope D-tracing experiments clarified the interaction among Brønsted acid of zeolite, water and methanol, confirming the proposed mechanism pathways. This work provides a facile new method for using H-Beta zeolite and MSA as potential high-performance acid promoters for EMC. Download: Download high-res image (136KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS A-PHYSICAL
·
2026
·
IF 5.1
Guan Yanfang,Zhang Qingyuan,Su Jiajun,Jian Yuhang,Wei Xinxin,Yang Xinlun,Zheying Wang,Yang Jinchu,Zhou Bei,Li Limin,Wang Jingxin,Yue Longwang,Shi Yingli
Flexible PEDOT:S-H/CNF paper biosensor enables noninvasive sweat glucose monitoring for wearable use. • 0.2:0.6 EDOT:S-Na₂S₂O₈ ratio yielded 17.08 S/cm conductivity, low swelling, and superior performance. • 3.ENS strategy enabled stable GOx covalent binding, enhancing activity and ensuring long-term stability. • 4.Optimized IDE geometry enhanced charge transfer, boosting sensitivity and lowering resistance. • 5.<5% glucose error in sweat across varied conditions enables real-time clinical monitoring. Biosensors enable disease, environmental, and metabolite monitoring due to high sensitivity, rapid response, and biocompatibility. However, wearable formats suffer from limited flexibility, inefficient enzyme immobilization, and poor wearability. Here, we present a wearable, stable, fast-responding sweat glucose (SG) biosensor using paper-based interdigitated electrodes (PIDE) coated with PEDOT:S-H/cellulose nanofiber (PSH/CNF,PCN) and covalently immobilized glucose oxidase (GOD). The composite exhibits high conductivity (17.08 S/cm), low swelling, and robustness; PSH is synthesized from EDOT:S and Na₂S₂O₈ (0.2:0.6) and mixed with CNF at 1:16 (v/v). The optimized PIDE geometry (1 mm spacing, 0.5 mm width, 10 mm length, 6 pairs) reduces interfacial impedance (180 Ω) and improves sensitivity (0.042 mA/mM). A one-sided GOD immobilization via 1-ethyl-(3-dimethylaminopropyl) carbodiimide hydrochloride/N-hydroxysuccinimide/succinic acid (EDC/NHS/SA, ENS) coupling yields ~2% enzyme leaching. The sensor shows a fast response (1.172 s) and peak current (0.1154 mA). Robust performance persists across pH 4–10, 36–39 °C, 3–5 mg/mL NaCl, and 30–70% RH. An SG concentration–impedance model (0.064–4.102 mmol/L) is established. Predicted SG trends deviate by <5% from blood glucose across five physiological states. The PIDE design enables better flexibility, integration and stability than conventional three-electrode sensors. This PIDE biosensor enables sensitive, stable noninvasive SG monitoring. Download: Download high-res image (167KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124471
·
IF 7.5
Sijun Chen,Yang Liu,Jingrong Liu,Tingwei Zhang,Yongcan Jin,Huining Xiao
Sulfonated carbon materials are promising heterogeneous Brønsted acid catalysts for biomass valorization, but the facile construction of carbon frameworks with accessible acid sites remains challenging. Herein, a sulfonated fructose-based porous nanosheet carbon (SPC) was synthesized via a facile and energy-efficient two-step strategy involving P 2 O 5 -assisted rapid self-propagating carbonization and concentrated sulfuric acid sulfonation, and subsequently employed for fructose dehydration to HMF in a low-boiling 1,4-dioxane/H 2 O solvent system. During carbonization, P 2 O 5 simultaneously promoted fructose carbonization and directed the formation of a porous nanosheet architecture, avoiding conventional high-temperature activation processes. The resulting porous nanosheets provided abundant sites for -SO 3 H grafting and enhanced Brønsted acid site accessibility. Consequently, SPC exhibited efficient catalytic performance for the selective dehydration of fructose, affording an HMF yield of 70.1% at 140 ℃ for 30 min. Moreover, SPC efficiently converted concentrated fructose (1.0 g fructose) to HMF with a 59.4% yield and exhibited moderate recyclability. This work provides a facile strategy for constructing biomass-derived sulfonated carbon solid acids with effectively utilized Brønsted acid sites for biomass upgrading.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）