JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Fenghao Yu,Chaoxin Qiu,Cong Xiao,Yanxin Du,Lin Lai,Wei Ren,Wei Li,Liting Jiang,Xiaohua Luo,Shengcan Ma
At present, Ag-based thermoelectric materials have received extensive attention and have demonstrated excellent performance in related device application. Among them, AgBiSe 2 is a lead-free thermoelectric material that exhibits significant n -type doping characteristics. It has been previously reported that R Cl 3 -doping ( R denotes the rare earth elements) has achieved excellent results in some n -type thermoelectric materials. However, there is still a lack of systematic research on the effect of R Cl 3 doping on AgBiSe 2 based materials. In this work, n -type AgBiSe 1.98 polycrystalline materials doped with CeCl 3 (0.5–2 mol%) are successfully synthesized by the melting method in combination with spark plasma sintering (SPS) technique. Compared with AgBiSe 2 , the CeCl 3 -doped AgBiSe 1.98 samples have achieved a significant increase in thermoelectric figure of merit ( ZT ) value, which should be attributed to the higher power factor ( PF = S 2 σ ) and inherently low thermal conductivity. Specifically, a large ZT max of ∼ 0.65 is achieved at 733 K in the 2 mol% CeCl 3 -doped AgBiSe 1.98 sample, which shows an increase of 41 %. This study demonstrates that CeCl 3 -doping, as a novel strategy that can improve simultaneously n H and m *, reveals excellent optimization effects in the thermoelectric performance regulation of AgBiSe 2 -based materials.
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POLYMER
·
2025
·
IF 4.5
Xiaoqiang Xue,Yangjing Chen,Xuepei Miao,Jian Liu,Yi Ding,Yuheng Zhang,Yunkai Sun,Wenyan Huang,Qimin Jiang,Hongting Pu
Environmentally sensitive polymer materials exhibit diverse properties due to their ability to respond to external environmental changes such as light, temperature, pH, and et al. These responses lead to corresponding alterations in their structure or state, resulting in unexpected performance. In this study, azo pyridine groups were introduced into the end groups and side chains of PNIPAM to synthesize two distinct polymer structures (PNIPAM-AZO and P (NIPAM- co -PAZO- co -OEGMA). This integration enables the polymers to respond to multiple stimuli, including temperature, light, pH, and gas (CO 2 ). A comprehensive investigation of the properties of these multi-responsive polymer materials was conducted. The findings reveal that the presence of azo pyridine units enables both polymers to modulate the (lower critical solution temperature) LCST of PNIPAM through UV, pH, and CO 2 , with a maximum temperature adjustment of 13 °C when CO 2 is introduced. This modulation range is influenced by the azo pyridine content in the polymer. Notably, when azo pyridine is present only at the polymer end group, the maximum LCST regulation range is limited to 3 °C. Moreover, the LCST of the two polymers can also be adjusted by pH. In the presence of carbonate ions, the protonation of azo pyridine by carbonic acid increases the solubility of the polymer and enhances the LCST. Introducing argon gas removes CO 2 , thereby restoring the polymer's solubility and LCST to their neutral condition levels. By alternately introducing CO 2 and argon gas, the LCST of the polymer exhibits cyclic changes.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2024
·
IF 3.9
Tingting Xiang,Qingchao Zhu,Tanyu Zhou,Chenglong Chen,Ruibo Wang,Tieyu Hu,Bing Li,Ziwei Xu,Juan Yang
Graphical Fe−N−C catalysts, doped with phosphorus, show improved ORR activity. Fe-NPC catalyst exhibits high metal loading, excellent ORR performance (onset potential of 1.00 V, half-wave potential of 0.864 V), and promising application in Zn-air batteries (758.8 mAh g −1 Zn ). DFT calculations reveal that phosphorus enhances O 2 activation and reduces the energy barrier for the rate-determining step. Atomically dispersed iron and nitrogen co-doped carbon materials (Fe−N−C) represent promising non-precious metal catalysts for the oxygen reduction reaction (ORR), offering potential alternatives to noble metal-based benchmarks. In our study, we investigated the influence of phosphorus doping on the catalytic activity of Fe−N−C. The experimental research demonstrate that the doping of phosphorus significantly enhances the ORR activity. Specifically, the resulting Fe-NPC exhibits high metal loading and excellent ORR activity in 0.1 M KOH with an onset potential of 1.00 V and a half-wave potential of 0.864 V. Density functional theory (DFT) simulations reveal that phosphorus improves the electrocatalytic activity by activating O2 molecules and reducing the energy barrier (the hydrogenation reaction *OH→H2O) of the rate-determining step. Furthermore, Fe-NPC exhibits promising application prospects as an air cathode in Zn-air batteries, delivering a high maximum discharge power density of 180.3 mW cm −2 and outstanding discharge specific capacity (758.8 mAh g −1 Zn ) at a discharge current density of 10 mA cm −2 .
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Chem
·
2024
·
IF 19.1
Xiaoran Zhang,Xiaorong Zhu,Shuowen Bo,Chen Chen,Qingfeng Zhai,Shuang Li,Xiaojin Tu,Jianyun Zheng,Dongdong Wang,Xiaoxiao Wei,Wei Chen,Tehua Wang,Yafei Li,Qinghua Liu,San Ping Jiang,Liming Dai,Shuangyin Wang
Electrocatalysis offers a sustainable approach to artificial nitrogen fixation yet faces numerous challenges. Selective synthesis of nitrogen-containing compounds shows promise but needs significant improvement. Herein, we demonstrate selective ammonia and urea synthesis via co-electrolysis with CO 2 . High CO binding energy on Re-Mn catalysts leads to the formation of ∗C species, which serve as electron reservoirs to enhance N 2 activation for C-N coupling (N 2 + ∗C → ∗CN 2 ), followed by C-N dissociation. This results in ammonia production with a yield rate of 48.9 ± 2.4 mg g −1 h −1 and an N-selectivity of 98.4%. In contrast, Zn-Mn sites, characterized by low CO binding, facilitate the migration of CO and its coupling with adsorbed N 2 (CO + ∗N=N∗ → ∗NCON∗). Subsequent hydrogenations of ∗NCON∗ promote urea synthesis with an N-selectivity of 89.1%. Utilizing Janus coupling with two C-N pathways aims to meet energy, agriculture, and chemical industry demands. We realized the selective synthesis of ammonia and urea, respectively, in one electrocatalytic system for the first time by Janus coupling with two distinguishable C-N coupling paths from N 2 and CO 2 .
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Biomass Conversion and Biorefinery
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2025
·
IF 4.1
Zhao Xiaoben,He Tao,Wang Shuainan,He Song
In this research, nitrogen-doped activated carbons (NACs) featuring a high specific surface area (3396 m 2 /g) and a certain amount of nitrogen doping (0.79–1.69%) were prepared by a combination of chemical activation and self-activation methods, and their CO 2 adsorption characteristics were comprehensively assessed. The experimental results showed that nitrogen doping not only significantly enhanced the specific surface area of the materials, but also significantly enhanced the CO 2 adsorption. The CO 2 adsorption capacity of the optimal sample, CMAC-0.5–3-700, reached 4.11 mmol/g and 2.32 mmol/g at 0 °C and 25 °C, respectively. In addition, the selectivity of NACs for CO 2 /N 2 was significantly improved, with a selectivity factor of up to 50.16, and the competitive adsorption experiments also demonstrated that NACs could still effectively adsorb CO 2 under the condition of CO 2 /N 2 = 15/85. Density-functional theory (DFT) calculations further revealed the interaction mechanism between NACs and CO 2 molecules, the enhanced CO 2 selectivity is attributed to electrostatic and π-electron interactions between nitrogen atoms and CO 2 . The findings indicate the significant potential of nitrogen-doped activated carbons (NACs) with high specific surface area and substantial nitrogen doping for post-combustion CO 2 capture.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yan Li,Huibin Liu,Mingyu Ma,Wenchao Peng,Yang Li,Xiaobin Fan
Vanadium-based oxides, known for their high capacity and low cost, have garnered significant attention as promising cathode candidates in aqueous zinc-ion batteries. Nonetheless, their poor rate performance and limited durability in aqueous electrolytes present a challenge to the realistic implementation of vanadium-based aqueous zinc-ion batteries. Here, we synthesized nitrogen-doped V2O3@C (N–V2O3@N–C) via ammonia treatment of V2O3@C derived from vanadium-based metal–organic framework (V-MOF), aiming to achieve outstanding rate and cycling performance. The N–V2O3@N–C electrode exhibits notable in situ self-transformation into an amorphous state. Density functional theory calculations reveal that the distorted N–V2O3 structure and uneven charge distribution result in the creation of an amorphous state. As expected, Zn/N–V2O3@N–C aqueous zinc-ion batteries can achieve remarkable specific capacity (349.0 mAh g–1 at 0.1 A g–1), along with impressive rate performance, showcasing a capacity of 253.5 mAh g–1 at 5 A g–1 and exceptional durability at 5 A g–1 (96.4% after 1350 cycles). The employed induced amorphization approach offers novel perspectives for designing high-performance cathodes that exhibit both sturdy structures and extended cycling lifespans.
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高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2024
·
IF 2
Xiaodong Shen,Yinde Zhang,Yanxia Li,Long Shen,Jialin Shi,Yang Li
Phase equilibria of carbon dioxide (CO2) hydrate in aqueous solutions of N-methyldiethanolamine (MDEA) at four different mass fractions (5, 10, 15, and 25 wt %) in the temperature range of 274.01 to 281.93 K and pressure range of 1.79 to 4.34 MPa were experimentally investigated by adopting an isochoric pressure search method. The reliability and accuracy of our experimental apparatus and method were examined by comparing the measured data with published ones. The enthalpy of CO2 hydrate dissociation was calculated by the Clausius–Clapeyron equation. The experimental results showed that MDEA acted as a thermodynamic inhibitor which could suppress the equilibrium line of CO2 hydrate to lower temperatures or higher pressures. The thermodynamic inhibition effect was enhanced after increasing the mass fraction. However, it was weaker than the conventional thermodynamic inhibitors of ethylene glycol (EG) and sodium chloride (NaCl). MDEA had synergistic inhibition effects with EG and NaCl, as their mixtures had stronger thermodynamic inhibition performance. The average enthalpies of CO2 hydrate dissociation in the presence of MDEA (5 to 25 wt %) were found to be in the range of 67.562 to 80.776 kJ·mol–1, which were very close to that of pure water. The research results have theoretical guidance for the flow assurance of natural gases.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Boyu Wang,Yani Huo,Cheng Chen,Xiao-Ye Wang,Chuancheng Jia,Jinying Wang,Xuefeng Guo
Achieving dynamic control over stereostructures and electronic properties of rigid molecules remains a significant challenge due to the delicate balance between stability and flexibility. Here, the construction of butterfly-shaped molecular junctions stabilized by moderate-strength boron-nitrogen (B←N) coordination between boraacenes and pyridines is reported. By leveraging the pivot-like flexibility of B←N bonds, molecular conductance switching with on/off ratios exceeding 100 is achieved through force-driven dynamic transitions between distinct stacking conformations. Single-molecule electrical measurements combined with first-principle calculations identify distinct charge transport mechanisms—through-space and through-bond—associated with the butterfly-wing open and closed configurations. Furthermore, external factors like electric fields and substituent effects modulate π – π interactions and charge transport properties. The introduction of destructive quantum interference effects can be achieved by replacing molecular units. The findings demonstrate that B←N coordination serves as a dynamically tunable linkage, offering a pathway to design molecular platforms with multifunctional units, customized stereo-conformations, and quantum effects.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jie Chen,Qiang Sun,Deyu Bao,Taoyi Liu,Wei-Di Liu,Can Liu,Jun Tang,Dali Zhou,Lei Yang,Zhi-Gang Chen
Owing to the intrinsically good near-room-temperature thermoelectric performance, β-Ag2Se has been considered as a promising alternative to n-type Bi2Te3 thermoelectric materials. Herein, we develop an energy- and time-efficient wet mechanical alloying and spark plasma sintering method to prepare porous β-Ag2Se with hierarchical structures including high-density pores, a metastable phase, nanosized grains, semi-coherent grain boundaries, high-density dislocations, and localized strains, leading to an ultralow lattice thermal conductivity of ∼0.35 W m–1 K–1 at 300 K. A relatively high carrier mobility is obtained by adjusting the sintering temperature to obtain pores with an average size of ∼260 nm, therefore resulting in a figure of merit, zT, of ∼0.7 at 300 K and ∼0.9 at 390 K. The single parabolic band model predicts that zT of such porous β-Ag2Se can reach ∼1.1 at 300 K if the carrier concentration can be tuned to ∼1 × 1018 cm–3, suggesting that β-Ag2Se can be a competitive candidate for room-temperature thermoelectric applications.
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Frontiers in Materials
·
2022
·
IF 3.985
Cao Ying,Li Wenjiao,Quan Fengyu,Xia Yanzhi,Xiong Zhong
Light-responsive hydrogel actuators show attractive biomedical applications for in vivo drug delivery tool, surgical tissue repair operation, and vascular cleaning due to its non-contact, rapid, precise, and remote spatial control of light. Conventional visible–light–responsive hydrogels contain special chemical structure or groups, and the difficulty in synthesis results in that few can be applied to fabricate visible–light–driven hydrogel actuators. In this study, based on photothermal effect, surface-modified Fe3O4 nanoparticles were incorporated into poly(N-isopropylacrylamide-acrylamide) hydrogel by UV photopolymerization, which revealed excellent green–light–responsive volume change. Under a laser irradiation of 200 mW at 520 nm, the bending angle deformation of hydrogel strips with 2.62 wt% Fe3O4 reached 107.8°. Strip-shaped hydrogel actuators could be applied to transport tiny objects. Furthermore, a boomerang-like hydrogel actuator was designed and fabricated to drive floating foam on water. By 12 cycles of continuous laser on–off irradiation to a hydrogel actuator underwater, a circular returning movement of the float was accomplished. The study on driving a float using visible–light–triggered hydrogel actuators provides a new idea for the design of light-driven biomedical devices and soft robots.
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Polymers
·
2020
·Vol. 12
·期 11
·2565
·
IF 3.426
Yiting Li,Lihui Zhang,Youhong Shi,Jialing Huang,Yaqiong Yang,Dengming Ming
Silicon nanocrystals (Si NCs) have received surging interest as a type of quantum dot (QD) due to the availability of silicon in nature, tunable fluorescence emission properties and excellent biocompatibility. More importantly, compared with many group II–VI and III–V based QDs, they have low toxicity. Here, thermoresponsive poly(N-isopropylacrylamide) (PNIPAAm)-functional Si NCs were firstly prepared for thermoresponsive detection of cancer cells. Si NCs were prepared under normal pressure with excellent water solubility. Then folic acid was bonded to the silicon nanocrystals through the reaction of amino and carboxyl groups for specific recognition of cancer cells. The folic-acid-modified silicon crystals (Si NCs-FA) could be modified by a one-pot copolymerization process into PNIPAAm nanospheres during the monomer polymerization process (i.e., Si NCs-FA-PNIPAAm) just by controlling the temperature below the lower critical solution temperature (LCST) and above the LCST. The results showed that the Si-FA-PNIAAm nanospheres exhibited not only reversible temperature-responsive on-off fluorescence properties, but also can be used as temperature indicators in cancer cells.Keywords:silicon nanocrystals;PNIPAAm;fluorescent imaging;thermoresponsive
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Song Wei,Caichao Wan,Luyu Zhang,Xinyi Liu,Wenyan Tian,Jiahui Su,Wenjie Cheng,Yiqiang Wu
Transition-metal oxides are a class of promising pseudo-capacitive materials for high energy density supercapacitors, while their low intrinsic conductivity, limited electrochemical sites and remarkable volume expansion deteriorate the electrochemical properties. Herein, we develop a facile synchronization strategy to prepare a N-doped and oxygen vacancy-rich NiCo 2 O 4 microporous nanograss (N–Ov–NCO MiNG), with adjustable superficial nanoporous architecture and electronic structure. Because of the instructive synergy of doping, defect, and surface-engineering achieved by one-step plasma activation, the optimum electrode (N–Ov–NCO MiNG–15) for supercapacitors exhibits significantly enhanced electrochemical properties, like an ultra-high specific capacitance of 2986.25F g −1 at 1 mA cm −2 and outstanding cyclic stability with a capacitance retention of 96.5% after cycling for 12,000 times. In addition, an aqueous asymmetric supercapacitor (ASC) device, assembled with the N–Ov–NCO MiNG–15 as the cathode and commercial activated carbon (AC) as the anode, shows an extremely high energy density of 103.2 Wh kg −1 at the power density of 748.3 W kg −1 , superior to most state-of-the-art supercapacitors and thus exhibiting a great potential in practical applications.
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