Nature Catalysis
·
2023
·Vol. 6
·期 2
·174-184
·
IF 37.8
Hua Wuxing,Shang Tongxin,Li Huan,Sun Yafei,Guo Yong,Xia Jingyi,Geng Chuannan,Hu Zhonghao,Peng Linkai,Han Zhiyuan,Zhang Chen,Lv Wei,Wan Ying
Understanding sulfur conversion chemistry is key to the development of sulfur-based high-energy-density batteries. However, unclear relationships between the electronic structure of the catalyst and its activity are the major problem. Here, we provide a direct correlation between the p electron gain of S in p -block metal sulfides and the apparent activation energies ( E a ) for the sulfur reduction reaction (SRR), in particular, Li 2 S n to Li 2 S conversion, which is the rate-determining step of the SRR. The maximum p charge occurs in bismuth sulfide and results in the lowest E a and a high SRR rate in the cathode. Li–S batteries with the Bi 2 S 3 catalyst work steadily at a high rate of 5.0C with a high-capacity retention of ~85% after 500 cycles. A high areal capacity of ~21.9 mAh cm −2 was obtained under a high sulfur loading of 17.6 mg cm −2 but a low electrolyte/sulfur ratio of 7.5 μl mg −1 .
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ACS Nano
·
2026
·
IF 16
Kuo Sun,Ningxin Xiao,Shaojian Jiang,Kai Deng,You Xu,Ziqiang Wang,Liang Wang,Hongjie Yu,Hongjing Wang
Electrocatalytic alkynol semihydrogenation (EASH) represents a promising alternative to conventional alkenol production. However, it is plagued by severe overhydrogenation and a competitive hydrogen evolution reaction (HER). In this work, we synthesize a Pd3BiCx intermetallic carbide metallene (Pd3BiCx ene) as a high-performance electrocatalyst for the selective semihydrogenation of 2-methyl-3-butyn-2-ol (MBY). At −0.3 V vs RHE, the catalyst system achieves 94.1% conversion, 95.3% selectivity, and 90.4% Faradaic efficiency while maintaining long-term stability over 70 h. Mechanistic studies demonstrate that carbon doping induces synergistic p-d-p orbital hybridization among Pd, Bi, and C. This electronic structure modulation optimizes the adsorption energy of MBY while facilitating the desorption of 2-methyl-3-buten-2-ol (MBE). Furthermore, carbon doping kinetically hinders overhydrogenation by eliminating subsurface hydrogen species and increasing the energy barrier for the overhydrogenation step. Concurrently, this p-d-p hybridization stabilizes surface adsorbed hydrogen (H*ads), thereby promoting the hydrogenation pathway and suppressing the HER. This work establishes an effective catalyst design strategy for fabricating p-d-p orbital-hybridized intermetallic catalysts, offering an innovative approach for high-efficiency EASH.
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 38
·21766-21773
·
IF 10.733
Shixue Zhang,Huan Liu,Bin Cao,Qizhen Zhu,Peng Zhang,Xin Zhang,Renjie Chen,Feng Wu,Bin Xu
Two-dimensional transition metal carbides (MXenes) have a unique structure, excellent electronic conductivity and a low Li+ diffusion barrier, and show potential for application in energy storage. Especially, MXenes can act as a conductive matrix to achieve excellent lithium storage performance. Herein, a Ti3C2Tx MXene/carbon nanotubes@red phosphorus (Ti3C2Tx/CNTs@P) nanohybrid with stable Ti–O–P bonds is fabricated. The CNTs are introduced into Ti3C2Tx to construct a conductive network, and then the Ti3C2Tx/CNTs are combined with P by a ball-milling method. In this process, the surface oxygen-containing functional groups of Ti3C2Tx interact with P, forming Ti–O–P bonds. Owing to the large capacity contribution of P, the conductive network and buffering role of Ti3C2Tx/CNTs, and the effect of the Ti–O–P bond, the Ti3C2Tx/CNTs@P nanohybrid exhibits a superior reversible capacity of 2598 mA h g−1 at 0.05C (1C = 2600 mA g−1, based on the active material P), excellent cycling stability (2078 mA h g−1 after 500 cycles) and superior rate capability (454 mA h g−1 at 30C). These results demonstrate that the Ti3C2Tx/CNTs@P nanohybrid offers fascinating potential for high-performance lithium-ion batteries.
研究领域:
材料科学
·
储能
·
纳米技术
·
电化学
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 47
·22672-22685
·
IF 3.925
Jing Wang,Mei Zhang,Feng Li,Huan Wang,Yanguang Chen,Hua Song
To deeply understand the role of P in hydrodeoxygenation (HDO), SiO2-supported Ni and Ni–P catalysts with different P/Ni ratios (x) were prepared. The as-prepared samples were characterized by various characterization methods. The HDO activity and product distribution over the Ni/SiO2 and N–P/SiO2-x were compared and the effects of x on the structure, acidity, formation mechanism of active phases and HDO performance were studied taking m-cresol HDO as a model reaction. The results showed that the introduction of P promotes the formation of smaller active sites and contributes to the creation of weak and medium strength acid sites through the formation of P–OH groups and Niδ+ in Ni2P. HDO over the Ni/SiO2 catalyst occurs mainly via the hydrogenation (HYD) route with 3-methyl-cyclohexanol (3-MCHnol) as the main product. However, for Ni–P/SiO2-x catalysts, methyl-cyclohexane (MCH) selectivity increases first and then decreases with the increase of x, reaching a maximum of 95% at x = 1. The acidity generated by the introduction of P contributes to increased MCH selectivity, while the dehydration of 3-MCHnol to MCH occurs mainly on acid sites. However, the excessively high P content (x ≥ 2.0) leads to a significant increase of MB (toluene) selectivity, which is associated with the increase in Ni(I) sites. About 100% m-cresol conversion was achieved with Ni–P/SiO2-1.0 when the m-cresol (g)/catalyst (g) ratio was 3, with MCH (99.4%) as the major product, showing great promise for deep HDO catalysis.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Pengna Wang,Ying Sun,Jie Li,Guanqun Zhu,Xueqin Zhang,Hong Yang,Baoping Lin
Novel monomer TPACz containing carbazole and triphenylamine active groups was synthesized. P(TPACz)/WO 3 coralloid porous electrochromic electrode material were prepared by electropolymerization . The P(TPACz)/WO 3 coralloid porous composite electrode material exhibited independent electrochromic properties in the positive potential range (0−1.7 V) (yellow at neutral state and blue at oxidation state) and negative potential range (−1.8−0 V) with the color of the film changing from yellow to dark blue. At the same time, the electrochemical properties of P(TPACz)/WO 3 composite material ware tested. It is noteworthy that the P(TPACz)/WO 3 coralloid porous electrochromic composite electrode materials exhibit both n-type and p-type doped electrochemical properties . Especially, P(TPACz)/WO 3 exhibit excellent capacitive properties in the n-doped state. According to its GCD curve of P(TPACz)/WO 3 nanocomposite electrode material, the area ratio capacitance is 1.94 mF cm −2 in the positive potential window of 0−0.8 V. And the area ratio capacitance is 33.3 mF cm −2 in the negative potential window of −1.8−0 V. Therefore, the design and effects of the nanocomposite material can broaden application range of electrochromic electrode materials and provide new strategies for energy saving material design.
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高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Huihua Wang,Wenchang Li,Jinhong Wu,Deyong Wang,Dong Hou,Minqi Sheng,Ruiqi Guo
Water splitting through electrolysis has been recognized as a promising solution for the production of hydrogen and oxygen to advance many renewable energy conversion and storage systems, while the key is the innovative exploration of cost-efficient electrocatalysts. Herein, interface-modified Ni–Fe–P/Co–P/NF alloys were achieved through a facile electroless plating strategy, in which the constructed interfaces benefited not only from the strong electron interaction but also from the fast mass transfer, significantly boosting the oxygen evolution reaction and hydrogen evolution reaction catalytic performance. More interestingly, water-splitting cells assembled using Ni–Fe–P/Co–P/NF-5L alloys as the cathode and anode, respectively, only requires a cell voltage of ∼1.52 V at 10 mA cm–2, far lower than that of the integrated Pt–C/NF and RuO2/NF couple (1.61 V). Also, the Ni–Fe–P/Co–P/NF-5L||Ni–Fe–P/Co–P/NF-5L system shows an outstanding durability over a long-term operation of 48 h at 10 mA cm–2. The work demonstrates an innovative strategy to construct heterogeneous interfaces for high-performance electrocatalysts and is suggested to be readily extended to regulate heterogeneous interfaces among other binary and ternary electrocatalysts, such as transition metal phosphides/borides, for scaling up water-splitting technology.
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高影响因子
DYES AND PIGMENTS
·
2024
·
IF 4.1
Di Wu,Yi Wang,Wenjing Qi,Jianyang Xu,Kanglin Pei,Lingyan Ma,Lin Qi
Long-lasting chemiluminescence of lucigenin/p-aminophenol (4-AP) system is explored for the first time and possible chemiluminescence enhancement mechanism is also proposed in this work. 4-AP can enhance chemiluminescence of lucigenin nearly 150 times and is stable for nearly 5 min, which overcomes the need of flow syringe pump. While o-aminophenol (2-AP) slightly enhances chemiluminescence of lucigenin and m-aminophenol (3-AP) does not. Thus, it can be applied in discrimination of three aminophenol isomers. More importantly, cyclic voltammetry proves the lowest oxidation peak for 4-AP at 115 mV, which is speculated to be the main reason for 4-AP induced chemiluminescence enhancement. It has been applied in chemiluminescence enhancement detection of 4-AP and p-nitrophenol (4-NP) from 80 nM to 60 μM, from 0.5 μM to 60 μM with limit of detection (LOD) of 26 nM and 0.17 μM, respectively. It shows high selectivity and anti-interference in chemiluminescence enhancment detection of 4-AP and 4-NP towards other organic compounds and metal ions. It also exhibits high accuracy in chemiluminescence enhancment detection of 4-AP and 4-NP in lake water with recoveries from 98.7% to 101.5% for and recoveries from 98.7% to 102.2%, respectively. It expands the study of long-lasting lucigenin chemiluminescence system and chemiluminescence method utilized in discrimination of aminophenols isomers.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Yimu Jiao,Qiyu Lian,Zhi Li,Muke Lin,Dingren Ma,Zhuoyun Tang,Dehua Xia,Mingshan Zhu
The p orbital electrons in main-group metals are generally underrated in the catalytic activity. Herein, an antimony (Sb) single-atom bipyridine-based covalent organic framework (SASb-TpBpy-COF) with the Sb─N coordination is successfully synthesized via 5p-2p orbitals hybridizarion for accomplishing the highly selective piezosynthesis of hydrogen peroxide (H 2 O 2 ) by the non-radical oxygen reduction reaction (ORR). Notably, the synthesized SASb-TpBpy-COF achieved an impressive H 2 O 2 piezosynthesis yield of 1500.58 µmol g −1 h −1 , which is up to more than 7-times higher than the reported catalysts. Moreover, the characterization results confirmed that the 5p-2p orbitals hybrid Sb single-atom can intrinsically drive the local polarization level, charge migration dynamics, electron-hole pairs separation, and affinity toward O 2 , consequently enhancing the piezoactivity and selective Pauling-type O 2 adsorption. Besides, experimental results clarified that the fast H 2 O 2 piezosynthesis is selectively dominated by the non-radical ORR. Furthermore, the dynamic Sb-OOH* intermediate is directly detected, proving the selective Pauling-type O 2 adsorption on the Sb single-atom sites. Moreover, this system can achieve an in situ degradation efficiency of over 80% for various emerging pollutants even in the real water samples. Conclusively, this study broadens the fundamental understanding for the fast H 2 O 2 piezosynthesis and provides a highly potential candidate technology for in situ water purification.
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高影响因子
ENVIRONMENTAL POLLUTION
·
2017
·
IF 5.099
Qian Liu,Wentao Shao,Chunlan Zhang,Cheng Xu,Qihan Wang,Hui Liu,Haidong Sun,Zhaoyan Jiang,Aihua Gu
Organochlorine pesticides (OCPs) can persistently accumulate in body and threaten human health. Bile acids and intestinal microbial metabolism have emerged as important signaling molecules in the host. However, knowledge on which intestinal microbiota and bile acids are modified by OCPs remains unclear. In this study, adult male C57BL/6 mice were exposed to p, p’-dichlorodiphenyldichloroethylene (p, p’-DDE) and β-hexachlorocyclohexane (β-HCH) for 8 weeks. The relative abundance and composition of various bacterial species were analyzed by 16S rRNA gene sequencing. Bile acid composition was analyzed by metabolomic analysis using UPLC-MS. The expression of genes involved in hepatic and enteric bile acids metabolism was measured by real-time PCR. Expression of genes in bile acids synthesis and transportation were measured in HepG2 cells incubated with p, p’-DDE and β-HCH. Our findings showed OCPs changed relative abundance and composition of intestinal microbiota, especially in enhanced Lactobacillus with bile salt hydrolase (BSH) activity. OCPs affected bile acid composition, enhanced hydrophobicity , decreased expression of genes on bile acid reabsorption in the terminal ileum and compensatory increased expression of genes on synthesis of bile acids in the liver. We demonstrated that chronic exposure of OCPs could impair intestinal microbiota; as a result, hepatic and enteric bile acid profiles and metabolism were influenced. The findings in this study draw our attention to the hazards of chronic OCPs exposure in modulating bile acid metabolism that might cause metabolic disorders and their potential to cause related diseases in human.
研究领域:
毒理学
·
微生物学
·
代谢组学
·
环境健康
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高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·10895
·
IF 15.7
Wang Wei,Wang Xinying,Yang Huanhuan,Yu Zhipeng,Zhang Weicai,Huang Haoliang,Zhao Zaowen,Zheng Xuerong,Liu Lifeng,Deng Yida,Li Yunyong
A rational design principle for selecting optimal anion dopants in transition-metal compounds to enhance sulfur redox activity is lacking in Li-S batteries. Herein, we propose an accurate p-p-s orbital electronic coupling descriptor (involving the p -orbitals of anion dopants and anions in transition-metal compounds and the s -orbitals of Li in lithium polysulfides) as a criterion for choosing anion dopants to guide the development of efficient anion-doped Li-S catalysts through machine-learning, theoretical, and experimental validation. We reveal the relationship between the electronic properties of various anion-doped WSe 2 and the thermodynamics and kinetics of sulfur redox. Our findings show that moderate p-p-s orbital electronic coupling optimizes polysulfide adsorption, facilitating Li 2 S nucleation and decomposition, thereby minimizing Gibbs free energy and maximizing catalytic efficiency for sulfur redox. A volcano relationship between the p-p-s coupling strength and catalytic activity is established. The optimal B-WSe 2 /MXene catalyst achieves a ~ 3 Ah pouch cell with 430 Wh kg −1 specific energy and good cycle life (81.3% capacity retention over 71 cycles). These findings provide a guideline for designing efficient anion-doped Li-S catalysts with moderate p-p-s coupling to enable rapid sulfur catalytic conversion in Li-S batteries.
研究领域:
材料科学
·
电化学
·
储能技术
·
催化
·
计算材料设计
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PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Wenxin Li,Bo Yu,Yang Hu,Xinqiang Wang,Bin Wang,Xiaojuan Zhang,Dongxu Yang,Zegao Wang,Yuanfu Chen
Exploring highly efficient, stable and nonprecious electrocatalysts for both hydrogen and oxygen evolutions is greatly desirable for sustainable energy conversion, but still a huge challenge. Herein, we construct a unique three-dimensional (3D) porous electrocatalyst with hollow (Co,Fe)P nanoframes encapsulated into N,P-codoped graphene aerogel (CFP NFs@NPGA) through one-step in situ encapsulation and selective etching, followed by phosphorization. Due to its uniqure 3D porous nanoarchitecture, CFP NFs@NPGA displays superior electrocatalytic performance. As a highly efficient catalyst for hydrogen evolution reaction , the CFP NFs@NPGA catalyst only needs low overpotential of 155 mV to afford 10 mA cm −2 under alkaline condition. Meanwhile, the hybrid reveals remarkable oxygen revolution reaction activity with a small overpotential of 278 mV to afford 10 mA cm −2 in alkaline electrolyte . When adopted as both cathode and anode in overall water-splitting cell, the hybrid requires only 1.59 V to achieve 10 mA cm −2 with nearly 100% faradaic efficiency, and the experimentally measured H 2 and O 2 gas genenaration rates are about 0.18 and 0.09 mmol h −1 , respectively, showing outstanding long-term stability even over 48 h. The present results manifest that the combination of hollow nanostructure and hetero-atom-doped carbon matrix is an effective strategy to enhance water-splitting performance of transition metal phosphides.
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高影响因子
JOURNAL OF POLYMER RESEARCH
·
2012
·Vol. 19
·期 11
·1-7
·
IF 1.733
Yu Wei-Na,Liu Shou-Xin,Wang Hong-Mei,Tian Rong
Temperature-responsive P(NIPAM- co -HMAM)- b -PEO- b -P(NIPAM- co -HMAM) triblock copolymers were synthesized by an atomic transfer radical polymerization (ATRP) method without freeze–pump–thaw cycles. The composition, structure, and molecular weight of the synthesized block copolymer were characterized by 1 H NMR and GPC. The phase transitions induced by temperature for different copolymers in dilute aqueous solutions have been studied using transmittance measurements, laser particle size measurements, viscosity analysis, and surface tension measurement, which showed that the HMAM content and the PEO (or PEG) chain length in the synthesized triblock copolymer affects the copolymer’s lower critical solution temperature (LCST). The micellization behavior of each temperature-responsive triblock copolymer was investigated by fluorescence probe measurements and transmission electron microscopy (TEM), which showed that the triblock copolymers form stable micelles above the LCST. The introduction of the HMAM component and the formation of micelles represent the first steps in the development of an injectable gel that forms in situ through chemical and physical crosslinking.
研究领域:
高分子化学
·
生物材料
·
药物递送系统
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高影响因子
危险品化学品经营许可证（带存储）