CHINESE JOURNAL OF CATALYSIS
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2024
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IF 15.7
Zhihan Yu,Dainan Zhang,Chenbing Ai,Jianjun Zhang,Quanjun Xiang
Accelerated charge migration and proton transfer to the reaction site are critical factors for improving photocatalytic efficiency. However, realizing both simultaneously is challenging because of the sluggish water (proton source) oxidation kinetics and interdependent redox reactions. Herein, we design an imide and hydrogen bond to connect carbon nitride ports of the D-π-A system with the dual-engineered linkages. The system uses an acetylene functional group and an imidazole ring as spatially separated water oxidation and oxygen reduction reaction (ORR) catalytic centers for photogenerated charge separation, respectively. The imine bond is a bridge grafted to the oxidation site to act as a hydrogen proton trap, and the hydrogen bond formed between reduction site and carbon nitride is used as the channel for instantaneous proton delivery to the reduction center. In situ characterization confirms that the linking sites protonation optimizes the pathway of ORR to H 2 O 2 and facilitates the *OOH intermediates generated. It is concluded that proton transport plays a critical role in optimizing photocatalytic H 2 O 2 production. Our work provides a strategy to improve dynamic proton transfer mechanisms.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Zhiguo Zhang,Hua Huo,Zhenjiang Yu,Lizhi Xiang,Bingxing Xie,Chunyu Du,Jiajun Wang,Geping Yin
Mn doping is deemed as a promising strategy to improve the electrochemical performance of the α-Ni(OH) 2 battery-type supercapacitor electrode. However, the internal structure evolution, the pathways and the dynamics of the proton/intercalated anion migration, as well as the functioning mechanism of Mn dopant to stabilize the layered structure during cycles remain unclear. Here, we unveil that irreversible oxidization of Mn 3+ at the initial CV cycles, which will remain as Mn 4+ in the NiO 2 slabs after the first oxidization to effectively suppress the phase transformation from α-Ni(OH) 2 /γ-NiOOH to β-Ni(OH) 2 /β-NiOOH and further maintain the structural integrity of electrode. With a synergistic combination of theoretical calculations and various structural probes including XRD and 2 H MAS solid state NMR, we decode the structure evolution and dynamics in the initial CV (cyclic voltammetry) cycles, including the absorption/desorption of hydrogen containing species, migration of intercalated anions/water molecules and the change of interlayer space. This present work elucidates a close relationship between doping chemistry and structural reliability, paving a novel way of reengineering supercapacitor electrode materials.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
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2014
·Vol. 44
·期 5
·2294-2298
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IF 4.097
Shanshan Man,Zenglong Wang,Boya Zhao,Lei Liu,Jinxiang Dong
Protic ionic liquids (PILs) are a subgroup of ionic liquids and easily formed by proton transfer from a Brønsted acid to a Brønsted base. Two new crystalline aluminophosphates, [C5H16N2][Al(PO4)(HPO4)] (AlPO-PIL1) and [C5H16N2][Al2(OH)2 (PO4)2] (AlPO-PIL2), are successfully prepared for the first time from a protic ionic liquid, 3-dimethylaminopropylamine acetate. Their structures were determined from single-crystal X-ray diffraction data. It was found that HF in the reaction mixture is crucial in determining the selectivity of the phase. In the absence of HF, AlPO-PIL1 with a one-dimensional chain structure was synthesized by templating the protonated 3-dimethylaminopropylamine cation of the PIL. Upon addition of HF to the initial reaction mixture, AlPO-PIL2 was obtained by templating the protonated N,N′-dimethyl-1,3-propanediamine, which was in situ generated from the protonated 3-dimethylaminopropylamine through migration of methyl groups during the crystallization. AlPO-PIL2 has a novel layered structure with a 3-connected 4·8·8 two-dimensional network which has never been found in the previously reported layered aluminophosphates.
研究领域:
材料化学
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晶体学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Lin Wang,Tao Wang,Yalong Li,Yi Huang,Rui Li,Jing Zhang,Jie Jiang,Pei Li,Yan Fan,Liang Chen
Multimodal sensors are devices characterized by their ability to respond in various ways and simultaneously detect and differentiate environmental changes, which is of significant importance for research on multifunctional wearable sensors. However, the majority of current studies on multimodal sensors struggle to incorporate simultaneous light intensity detection. This paper presents a novel approach that utilizes graphene oxide to create bilayer films with varying oxygen content using a thermal reduction process, enabling simultaneous detection and differentiation of ultraviolet light, humidity, and temperature, while demonstrating excellent flexibility and self-powered capabilities. The proposed structure reveals that the oxygen functional groups within graphene oxide can induce proton generation in response to external environmental stimuli, facilitating rapid proton migration driven by the asymmetric charge distribution resulting from the variation in oxygen content between the bilayer films. This innovative operational mechanism may provide new insights for implementing electrical signal transmission using protons as charge carriers. Furthermore, this structure holds potential for the design of artificial electronic skin and other wearable devices, enabling rapid detection of multiple signals in complex environments.
研究领域:
材料科学
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传感器技术
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生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
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2024
·Vol. 11
·期 16
·5014-5025
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IF 6.1
Xinyue Geng,Gaoqing Hang,Alberto J. Fernández-Carrión,Xing Ming,Sihao Deng,Lunhua He,Xiaojun Kuang,Xiaoyan Yang
Solid-state oxide ion and proton conductors are garnering significant attention due to their high ionic conductivity and potential applications in a range of electrochemical devices, including solid oxide fuel cells and gas sensors. In this study, we report the influence of partial substitution of La3+ in isolated tetrahedral LaVO4 ceramics with 0.01 mol of alkaline-earth metals Ca2+, Sr2+ and Ba2+ on the phase stability and electrical properties. It was found that acceptor doping effectively enhances mixed oxide ion and proton conductivities, with Sr2+ substitution yielding the highest conductivity, achieving ∼10−3 S cm−1 at 900 °C under a wet O2 atmosphere. DFT calculations and ab initio molecular dynamics simulations revealed that protons preferentially form hydrogen bonds with the lattice oxygen near the dopants and migrate through a continuous process of hopping and rotation between inter- and intra-tetrahedral VO4 groups. Additionally, the existence of oxygen vacancies facilitates the formation of V2O7 dimers through sharing corners with adjacent isolated VO4 tetrahedra, enabling ion exchange through a synergistic mechanism involving V2O7 dimer breaking and reforming. This research highlights the critical role of the deformation and rotational flexibility of isolated tetrahedral units in facilitating oxide ion and proton transport, underscoring the potential for developing mixed oxide ion and proton conductors in oxygen vacancy-deficient oxides with tetrahedral-based structures.
研究领域:
材料科学
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计算化学
✓ 已验证
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2024
·
IF 8
Lan Zhao,Qiqi Hong,Ningning Tan,Xinda You,Biao Huang,Beili Lu,Jianhua Lv,Lirong Tang
Heterostructures comprising zero–dimensional (0D) nanoparticles and two–dimensional (2D) nanosheets have garnered considerable interest for sensing applications. Guanine exhibits extraordinary functionality in terms of their abundant hydrogen bond donors/acceptors. In this study, the protonated amine matrix of guanine serves as augmented active sites, uniformly forming guanine nanoparticles (GN) between 2D vermiculite nanosheets (VMT) confined space. Through electrostatic interactions and cross–linking with heptanedioic acid (HA), a self–assembly heterostructure (GN/VMT–HA) was constructed, which may offer abundant transport channels for enhanced humidity sensing and proton migrations. The proton migrations of GN/VMT–HA increased from 0.585 mS/cm (11% RH) to 0.750 mS/cm (97%RH) at 25 °C. The humidity sensor based on GN/VMT–HA demonstrates excellent performance, including high sensitivity (30.20 Hz/%RH), small hysteresis (1.45% RH) and short response/recovery time (25 s/7 s). This study offers a simple green method for constructing 0D/2D nanocomposites for proton transfer and humidity–sensing applications.
研究领域:
材料科学
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传感器技术
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Gaopeng Zhou,Ying Li,Yadan Luo,Xi Wang,Yushi Ding
In this article, the structure and electrical properties of BaSn 0.15 Ce 0.35 Hf 0.25 Y 0.1 Yb 0.1 Ho 0.05 O 3-δ (referred as BSCHYYbHo in forthcoming discuss) high-entropy ceramic have been investigated. The BCHYYb (short for BaCe 0.5 Hf 0.3 Y 0.1 Yb 0.1 O 3-δ ) and BSCHYYbHo pellets were synthesized successfully by the solid-state reaction method. The XRD detection results indicate that there is no secondary phase appeared in BSCHYYbHo and the lattice constant decrease compared to BCHYYb. The surface SEM and EDS images illustrates that BSCHYYbHo is denser than BCHYYb and the elements distribution is more uniform. The DFT calculation proves that BSCHYYbHo has a tend to maintain single phase structure. The electrical properties of BSCHYYbHo is obtained by the DRT analysis and equivalent circuit method based on defect equilibria model. The total conductivity of BSCHYYbHo is about 2.02 × 10 -4 ∼1.01 × 10 -2 S·cm -1 and standard molar hydration enthalpy of BSCHYYbHo is recorded as − 81.8 kJ/mol. Further, the proton, oxygen vacancies and electron holes conductivity activation energies in BSCHYYbHo is estimated to be 0.45 eV, 1.41 eV and 1.60 eV, respectively. Compared to BCHYYb, BSCHYYbHo electrolyte has higher proton concentration and proton transference number. Overall, BSCHYYbHo ceramic with dense structure and high proton transference number is a potential material for application.
研究领域:
材料科学
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电化学
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陶瓷
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固体化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·Vol. 20
·期 26
·2310226
·
IF 13
Zhongwei Man,Zheng Lv,Yangyang Cao,Zhenzhen Xu,Qing Liao,Jiannian Yao,Feng Teng,Aiwei Tang,Hongbing Fu
Organic afterglow materials have significant applications in information security and flexible electronic devices with unique optical properties. It is vital but challenging to develop organic afterglow materials possessing controlled output with multi-stimuli-responsive capacity. Herein, dimethyl terephthalate (DTT) is introduced as a strong proton acceptor. The migration direction of N─H protons on two compounds Hs can be regulated by altering the excitation wavelength (Ex) or amine stimulation, thereby achieving dual-stimuli-responsive afterglow emission. When the Ex is below 300 nm, protons migrate to S 1-2 DTT , where strong interactions induce phosphorescent emission of Hs , resulting in afterglow behavior. Conversely, when the Ex is above 300 nm, protons interact with the S 0 DTT weakly and the afterglow disappears. In view of amine-based compounds with higher proton accepting capabilities, it can snatch proton from S 1-2 DTT and redirect the proton flow toward amine, effectively suppressing the afterglow but obtaining a new redshifted fluorescence emission with Δλ over 200 nm due to the high polarity of amine. Moreover, it is successfully demonstrated that the applications of dual-stimuli-responsive organic afterglow materials in information encryption based on the systematic excitation-wavelength-dependent (Ex-De) behavior and amine selectivity detection.
研究领域:
材料科学
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光学材料
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刺激响应材料
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信息加密
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物理化学
✓ 已验证
DOI
高影响因子
Journal of Energy Chemistry
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2025
·
IF 14.9
Zhan Zhao,Tao Shi,Jia Liang,Kelei Huang,Xiangchao Meng
Acceleration of hydrogen spillover on electrocatalysts is effective for improving the hydrogen evolution reaction. However, it is still challenging to design rational proton migration pathway. Herein, we propose an in-situ reconstruction strategy to provide MoO 4 2− -modified micro-environment, which prominently promotes the hydrogen spillover effect. The Mo species is introduced to be in situ oxidized and transformed to MoO 4 2− . Experimental and theoretical studies indicate that the generation and re-adsorption of MoO 4 2− not only suppress the interfacial electron accumulation, but also optimize the electronic structure to facilitate thermo-neutral adsorption of H*, thus forming the effective hydrogen spillover channel. Finally, the reconstructed catalyst exhibits excellent HER performance (overpotential of 183 mV at 1000 mA cm −2 in alkaline solution) and sustained high stability for 1000 h at 1000 mA cm −2 , which also shows great promising prospects for practical applications ( E W : 4.09 kW h m −3 ; η ETH : 86%@60 ℃) in anion exchange membrane alkaline water electrolyzer.
研究领域:
电化学
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催化
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能量转换
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材料科学
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纳米技术
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Hu Bai,Zhizhong Leng,Ting Chen,Bo Zhang,Jiaming Chu,Yanhong Zhang,Qi Zhou,Juan Zhou,Shaorong Wang
As clean energy conversion devices with the functions of power generation and hydrogen evolution , solid oxide cells (SOCs) are facing the obstacle of insufficient catalytic activity of traditional electrode materials under the trend of lower operation temperature . Here a double-perovskite material PrBa 0.5 Sr 0·5 Co 2-x Fe x O 5+δ (PBSCF, x = 0.5, 1.0, 1.5, 2.0) is reported and its application as oxygen electrode of symmetrical cells on the proton conductor BaZr 0·1 Ce 0·7 Y 0.1 Yb 0.1 O 3-δ (BZCYYb1711) is investigated. The tests are carried out under atmospheres with different water content (0, 20% and 40%), showing the influence of Fe/Co molar ratio on the crystal structure, conductivity, electrochemical properties and micro morphology of PBSCF series materials. With the increasing of Fe substitution content, the polarization resistance of PBSCF series symmetrical cells decreases. PrBa 0.5 Sr 0.5 Co 1.5 Fe 0.5 O 5+δ (PBSCF05) symmetrical cell always shows the optimal performance and exhibits area-specific polarization resistance (ASR) of 0.08 Ω cm 2 at 700 °C under 20%H 2 O+80%air. Further experimental results and the distribution of relaxation times (DRT) analysis show that the presence of an appropriate amount of steam in atmosphere would optimize the conductive mechanism and promote proton migration, while the presence of excessive steam would hinder the diffusion of oxygen molecule. For the electrochemical reaction on the PBSCF electrode, the adsorption, dissociation and precipitation of oxygen are always the crucial rate-limiting steps, which is a direction worthy of further optimization.
研究领域:
材料科学
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电化学
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能源转换
·
固体化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Lingfei Liu,Mingshan Zhang,Yi Lu,Gaojian Chen,Binda Lu,Lingling Ge,Zhouguang Lu,Dejun Sun,Zhenghe Xu
CO 2 -responsive microemulsion (ME) is considered a promising candidate for deep-cleaning and oil recovery from oil-contaminated soils. Understanding the responsive nature of different microstructures ( i.e. , oil-in-water (O/W), bicontinuous (B.C.) and water-in-oil (W/O)) is essential for unlocking the potential and mechanisms of CO 2 -responsive emulsions in complex multiphase systems and providing comprehensive guidance for remediation of oil-contaminated soils. Herein, the responsiveness of microstructures of ME to CO 2 trigger was investigated using experimental designs and coarse-grained molecular dynamic simulations. MEs were formed for the first time by a weakly associated pseudo-Gemini surfactant of indigenous organic acids (naphthenic acids, NAs are a class of natural surface-active molecules in crude oil) and tetraethylenepentamine (TEPA) through fine tuning of co-solvent of dodecyl benzene sulfonic acid (DBSA) and butanol. The O/W ME exhibited an optimal CO 2 -responsive character due to easier proton migration in the continuous aqueous phase and more pronounced dependence of configuration on deprotonated NA ions. Conversely, the ME with W/O microstructure exhibited a weak to none responsive characteristic, most likely attributed to its high viscosity and strong oil-NA interactions. The O/W ME also showed superior cleaning efficiency and oil recovery from oil-contaminated soils. The results from this study provide insights for the design of CO 2 -responsive MEs with desired performance and guidance for choosing the favorable operating conditions in various industrial applications, such as oily solid waste treatment , enhanced oil recovery (EOR), and pipeline transportation. The insights from this work allow more efficient and tailored design of switchable MEs for manufacturing advanced responsive materials in various industrial sectors and formulation of household products.
研究领域:
环境科学
·
化学工程
·
材料科学
·
表面化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）