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Small · 2025 ·Vol. 21 ·期 27 ·2412833 · IF 12.1

Orbital Splitting and Interstitial Doping Lead to High Thermoelectric Performance in n-type PbSe

Deshang Xiang,Yaru Gong,Chen Chen,Rongxin Sun,Song Zhao,Yuqi Liu,Qingyang Jian,Yanan Li,Wei Dou,Di Li,Pan Ying,Guodong Tang

PbSe has garnered significant attention due to its earth-abundance and low cost of Se element. Here the synthesis of Zn and Sn co-doped n -type PbSe with noteworthy thermoelectric performance enhancement is reported. Microstructural characterization and first-principles calculations demonstrate that Zn occupies the interstitial site between Se tetrahedra in PbSe, thereby creating a high-density network of needle-like defects that induces lattice strain and reduces the lattice thermal conductivity. Zn interstitial doping provides additional free electrons, leading to sharp increase of carrier concentration. DFT calculation reveals that orbital splitting of VBM boosts carrier mobility of PbSe. The significantly enhanced carrier mobility produces high power factor in the whole temperature range. As a result, a high peak ZT of 1.7 is realized for Zn and Sn co-doped n -type PbSe with a remarkable average ZT of 1.2 over the temperature range of 423–873K. These findings demonstrate that combining orbital splitting and interstitial doping is an effective strategy to synergistically optimize the electrical-thermal transport of n -type PbSe, making it a promising candidate for energy conversion applications.

研究领域: 材料科学 · 凝聚态物理 · 能源材料 · 热电转换 · 半导体物理
✓ 已验证 产品关联 DOI PubMed 高影响因子
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2017 ·Vol. 19 ·期 40 ·27221-27232 · IF 4.123

Two-step volume phase transition mechanism of poly(N-vinylcaprolactam) hydrogel online-tracked by two-dimensional correlation spectroscopy

Gehong Su,Tao Zhou,Xifei Liu,Yulin Zhang

In this study, temperature-dependent FTIR spectroscopy in combination with the perturbation–correlation moving-window (PCMW2D) technique and generalized two-dimensional (2D) correlation analysis was applied to investigate the phase transition mechanism of poly(N-vinylcaprolactam) (PVCL) hydrogel upon heating. In the conventional 1D FTIR spectra, the gradual dehydration of C–H groups, as well as the gradual dissociation of hydrogen bonds between CO groups and water molecules, was observed during phase transition. Moreover, we found that the rate at which water molecules were expelled out of the gel network during phase transition was changed to a sigmoid mode, rather than increasing linearly with increasing temperature. PCMW2D FTIR spectra revealed that the phase transition of PVCL hydrogel can be divided into two steps (named as I and II) upon heating, and we further determined the temperature regions of steps I and II to be 29.0–35.7 °C and 35.7–47.5 °C, respectively. Step I is the formation of hydrophobic domains in the gel, and step II is the chain collapse of the gel. Finally, with the help of generalized 2D correlation analysis, it was confirmed that the transformation of hydrogen bonds was the driving force of the hydrophobic domain formation process, while the hydrophobic interaction of C–H groups was the driving force for the chain collapse process. Combined with the obtained sequential orders of step I and step II, an integrated two-step phase transition mechanism of PVCL hydrogel upon heating was proposed.

研究领域: 材料科学 · 化学
✓ 已验证 DOI PubMed 高影响因子
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NEW JOURNAL OF CHEMISTRY · 2018 ·Vol. 43 ·期 2 ·820-826 · IF 3.201

Electrochemical sensor for facile detection of trace N-nitrosodiphenylamine based on poly(diallyldimethylammonium chloride)-stabilized graphene/platinum nanoparticles

Xiuying Peng,Jinfeng Zou,Zhiguang Liu,Yujing Guo

N-Nitrosodiphenylamine (NDPhA), a typically nonvolatile N-nitrosamine (NA), is widely used as an additive in daily human necessities and is considered as a possible cancer-causing substance by the US Environmental Protection Agency. Therefore, the determination of NDPhA in environment is crucial to people's health. In this study, a simple and high-performance electrochemical sensor for NDPhA detection is constructed based on poly(diallyldimethylammonium chloride)-stabilized graphene/platinum nanoparticles (PDDA–Gr/PtNPs) as an electrochemical sensing platform. The PDDA–Gr/PtNP nanocomposite is synthesized by a facile wet-chemical approach. It combines the prominent properties of graphene (large surface areas and high conductivity) with the outstanding catalytic activity of Pt nanoparticles. Because of its remarkable synergistic effect, a PDDA–Gr/PtNP-modified glassy carbon electrode (PDDA–Gr/PtNPs/GCE) shows excellent performance towards electrooxidation of NDPhA with a significantly increased peak current and negatively shifted peak potential compared to graphene-modified electrode (PDDA–Gr/GCE); it exhibits good linearity for NDPhA detection with a linear range of 1.0 × 10−7–5.0 × 10−5 mol L−1 and a detection limit of 3.3 × 10−8 mol L−1 (S/N = 3) under optimum conditions. Moreover, this cost-effective and convenient sensor also has good stability, repeatability and anti-interference ability and is promising for trace analysis of NAs in environmental pollutants.

研究领域: 环境科学 · 分析化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2025 · IF 3.9

N-Heterocyclic Carbene-Capped Highly Dispersed Pt Nanoparticles for Catalytic Dehydrogenation-Cracking of Decalin toward High Heat Sink

Junpeng He,Ruiqing Zhang,Xi Chen,Bofeng Zhang,Guozhu Liu

Active fuel cooling is an effective way to overcome the thermal barrier for hypersonic flight. Pt-based nanofluid catalysts are effective in enhancing the chemical heat sink of endothermic hydrocarbon fuels (EHFs) by facilitating a catalytic dehydrogenation-cracking reaction. However, highly-dispersed Pt nanoparticles often face the problem of poor thermal stability in nanofluids. In this work, a NaH-assisted deprotonation method was applied to synthesize N-heterocyclic carbene (NHC)-capped highly-dispersed Pt nanoparticles (Pt@NHC14). The average size of the Pt nanoparticles in optimized Pt@NHC14 was 2.4 nm. Pt@NHC14 exhibited a high heat sink of 3.80 MJ/kg at 725 °C in the quasi-homogeneous conversion of decalin, which was 10% higher than Pt@ILs14 without a deprotonation strategy. This could be ascribed to the dehydrogenation process being promoted, which was verified by a hydrogen yield of 9.5% on highly dispersed Pt of Pt@NHC14, and that is 46% higher than that of Pt@ILs14. This research synthesizes N-heterocyclic carbene-capped highly-dispersed Pt nanoparticles and provides valuable insights into the strong endothermic technology.

CAS / MDL: 16940-66-2
研究领域: 材料科学 · 化学工程 · 航空航天工程
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MICROCHEMICAL JOURNAL · 2020 · IF 3.594

Detection of residual formaldehyde in N-butyl-2-cyanoacrylate by high-performance liquid chromatography with rhodamine B hydrazide

Bokai Ma,Fujian Xu,Mian He,Yuqing Lin,Guanghui Hu,Mei Zhang,Xinying Zhao,Weili Liu

Rhodamine B hydrazide (RBH) was prepared as a new derivatizing reagent for residual formaldehyde in a drug such as N-butyl-2-cyanoacrylate (NBCA). RBH reacted with formaldehyde rapidly at room temperature, and the resulting derivative can be detected sensitively at 238 nm. After optimizing the derivatization and chromatographic separation conditions, RBH as a pre-column derivatizing reagent has been successfully used for the analysis of formaldehyde in real NBCA samples by high-performance liquid chromatography (HPLC). The detection limit of the method is 0.004 μg/mL for formaldehyde, and the recovery is 94.0%-96.6%. Most notably, compared with the previous HPLC methods, the developed method has the advantages of mild derivatization temperature, short derivatization time and high sensitivity.

研究领域: 分析化学 · 药物分析
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CERAMICS INTERNATIONAL · 2019 · IF 3.45

Enhanced n→π* electron transition of porous P-doped g-C3N4 nanosheets for improved photocatalytic H2 evolution performance

Chunyan Su,Yazhou Zhou,Lili Zhang,Xiaohui Yu,Shuai Gao,Xiujuan Sun,Chao Cheng,Qinqin Liu,Juan Yang

Graphitic carbon nitride (g-C 3 N 4 ) has been demonstrated to be a rising star among semiconductor materials for photocatalytic hydrogen (H 2 ) production. However, pristine g-C 3 N 4 usually suffers from inferior activity due to the inadequate visible light harvesting capacity and quick charge recombination. Herein, porous P doped g-C 3 N 4 nanosheets (PCNNSs) were fabricated via a simple thermal condensation of adenosine phosphate and urea followed by thermal exfoliation method. The synergetic effect of the porous structure and P dopant can provide abundant active sites for the photocatalytic reaction, which can enhance light absorption range extending from 450 nm to 700 nm attributed to the n→π* electronic transition, and improve hydrophilicity for easier water molecules adsorption via introducing hydroxyl groups. Furthermore, impurity level caused by the P dopant would change the excitation process and accelerate the charge separation efficiency. Therefore, the PCNNSs exhibited significantly elevated photocatalytic H 2 generation performance (9523.7 μmolg -1 h -1 ) under visible-light (λ > 420 nm) irradiation, which was about 20 times that of unmodified g-C 3 N 4 (458 μmol -1 h -1 ).

研究领域: 材料科学 · 能源化学
✓ 已验证 DOI 高影响因子
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Catalysts · 2019 ·Vol. 9 ·期 2 ·114 · IF 3.444

Ternary N, S, and P-Doped Hollow Carbon Spheres Derived from Polyphosphazene as Pd Supports for Ethanol Oxidation Reaction

Ke Yu,Yan Lin,Jinchen Fan,Qiaoxia Li,Penghui Shi,Qunjie Xu,Yulin Min

Ethanol oxidation reaction (EOR) is an important electrode reaction in ethanol fuel cells. However, there are many problems with commercial ethanol oxidation electrocatalysts today, such as poor durability, poor anti-CO poisoning ability, and low selectivity for C–C bond cleavage. Therefore, it is very meaningful to develop a high-performance EOR catalyst. Herein, we designed ternary N, S, and P-doped hollow carbon spheres (C–N,P,S) from polyphosphazene (PCCP) as Pd supports for EOR. Using SiO2spheres as the templates, the PCCP was first coated on the surfaces of SiO2spheres by in situ polymerization. Through high-temperature pyrolysis and hydrofluoric acid-etching, the hollow PCCP has a large surface area and porous structure. After loading Pd nanoparticles (NPs), the Pd/C–N, P, S catalysts with Pd NPs decorated on the surfaces of C–N, P, S can achieve a high mass peak current density of 1686 mA mgPd−1, which was 2.8 times greater than that of Pd/C. Meanwhile, the Pd/C–N, P, S catalyst also shows a better stability than that of Pd/C after a durability test of 3600s.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Zn–N bonds boost interfacial charge transfer in ZnO/Nitrogen-Doped porous carbon Schottky heterojunction for enhanced photocatalytic sterilization

Yangyang Sun,Shaosheng Rao,Qinqin Liu,Chuang Zhi,Zhongxi Lu,Rong Ma,Zhongti Sun,Juan Yang

Although heterogeneous photocatalytic sterilization can avoid secondary pollution and achieve broad spectrum antibacterial effects, its low disinfection efficiency seriously hinders its development. Exploring and achieving precise electron-transfer channels in the interface of heterogeneous systems are an effective method to enhance photocatalytic sterilization. Herein, we designed a chemical Zn–N bonded nitrogen-doped porous carbon-loaded zinc oxide (ZnO/NC) Schottky heterojunction photocatalyst through oxidizing and carbonizing ZIF-8 in-situ at suitable temperatures. The Zn–N accurately facilitated the photogenerated electrons transfer from the conduction band (CB) site of ZnO to the NC surface as active site. Furthermore, the NC as carrier enhanced the light-absorption capacity (746 nm) of Schottky heterojunction and functioned as active site to promote the generation of reactive oxygen species (ROS). In addition, the slow-release effect of zinc ions (Zn 2+ ) from ZnO contributed to the accelerated death of bacteria. As a result, under simulated sunlight conditions, the ZnO/NC-400(1 h) Schottky heterojunction demonstrated an impressive antibacterial efficiency of 99.33 % against Escherichia coli , consistently exceeding 95 % in repeated experiments. This work presents a controllable and encouraging approach for constructing heterojunction with effective antibacterial properties.

研究领域: 材料科学 · 环境科学 · 微生物学
✓ 已验证 DOI 高影响因子
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Microstructures · 2025 ·Vol. 5 ·期 1 ·N · IF 9

High-pressure modulation of band gap and microstructure in N-type high-entropy strontium titanate for enhanced thermoelectric performance

Xinjian Li,Xiaohuan Luo,Moran Wang,Tu Lyu,Chaohua Zhang,Fusheng Liu,Hongan Ma,Lipeng Hu

In thermoelectrics, optimizing both carrier and phonon transport is crucial for enhancing thermoelectric performance. Strontium titanate, a representative N-type oxide thermoelectric material, often exhibits inferior figure of merit (zT) due to its large band gap that limits carrier concentration, and high lattice thermal conductivity, attributed to strong Ti-O covalent bonds. Conventional approaches, such as aliovalent doping to increase carrier concentration or introducing structural defects to reduce lattice thermal conductivity, are insufficient as they fail to decouple the interdependent electrical and thermal properties. Herein, we introduce a high-pressure synthesis technique that concurrently modulates both the band gap and microstructure. This approach effectively enhances the carrier concentration by narrowing the band gap and increases the effective mass of the density of states through enhanced solubility limit of rare earth elements, significantly improving the power factor. Additionally, high-pressure condition induces microstructural defects, including point defects, dislocations, lattice distortions, and nanoscale grains, which promote broad-wavelength phonon scattering and minimize lattice thermal conductivity. Consequently, a peak zT value of 0.25 at 973 K is attained in high-entropy (Sr0.2La0.2Nd0.2Sm0.2Eu0.2)TiO3 synthesized at 5 GPa, representing a 5.3-fold improvement over undoped strontium titanate. This work highlights the pivotal role of high-pressure synthesis in decoupling the carrier and phonon transport in thermoelectrics.

研究领域: 材料科学 · 凝聚态物理 · 能源技术
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Enhanced moisture-resistance and excellent photocatalytic performance of synchronous N/Zn-decorated MIL-125(Ti) for vaporous acetaldehyde degradation

Zhu Gao,Jiaxing Wang,Yaseen Muhammad,Yibo Zhang,Syed Jalil Shah,Yang Hu,Zhe Chu,Zhongxing Zhao,Zhenxia Zhao

High photo-catalytic activity and stable recycling performance under high humidity are main hindering factors in practical applications of metal organic frameworks (MOFs) for volatile organic compounds (VOCs) degradation. In-situ co-doping strategy of pyrrolic N/Zn was proposed to enhance surface charge separation and cycling stability of MIL-125(Ti) for degradation of vaporous acetaldehyde under highly humid conditions. Characterizations results show that pyrrolic N/Zn co-doped MIL-125(Ti) exhibited an integrated crystal structure and high surface area (1415 m 2 /g). The constructed Ti/Zn-N/O clusters narrowed band gap (from 3.40 to 1.85 eV) of MIL-125(Ti) and boosted electron conductivity. Also, it was proved to enhance surface alkalinity and hydrophobicity of MIL-125(Ti), which would strengthen MOFs selective adsorption towards CH 3 CHO and accelerated the transfer of degradation product CO 2 from catalytic active sites in MIL-125(Ti) under high humidity. As a result, synergistic effect of N/Zn co-doping exhibited an enhanced the ability of activating oxygen and H 2 O molecules into superoxide radical ( O 2 − ) and hydroxy radical ( OH), showing 10 times faster reaction kinetics for CH 3 CHO degradation under humid air compared to MIL-125(Ti). Moreover, co-dopant of N/Zn into MIL-125(Ti) has significantly promoted the recycling stability of MIL-125(Ti) under high humidity. According to the work, co-dopant elemental strategy to modify MOF surface can provide the synergistic effect for efficient degradation of aldehyde VOCs under humid conditions.

研究领域: 材料科学 · 环境科学
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ACS Applied Energy Materials · 2022 · IF 6.959

In Situ Derivatization of NiAl-LDH/NiS a p–n Heterojunction for Efficient Photocatalytic Hydrogen Evolution

Youlin Wu,Pengfei Zhu,Youji Li,Lijun Zhang,Zhiliang Jin

Owing to the creation of a large number of surface active sites, surface modification is an efficient strategy for improving the catalytic performances of photocatalysts. Herein, zero-dimensional (0D) p-type NiS species were developed in situ on the large surface of NiAl-LDH by controlled vulcanization. Importantly, the development of the 0D p-type NiS species not only enriched the active sites but also triggered the in situ formation of a NiS/NiAl-LDH p–n heterojunction due to NiAl-LDH, which was utterly underdeveloped in the vulcanization modification procedure. This undoubtedly accelerated the faster separation and migration of charge carriers and yielded improved photocatalytic hydrogen evolution. The optimum hydrogen production rate of the NiS/NiAl-LDH photocatalyst could reach 3408 μmol·g–1·h–1 using a 5 W LED simulation visible light, which was 52-fold that of NiAl-LDH. The design and construction of the in situ p–n heterojunction may provide a perspective for the formation of p–n heterojunction photocatalysts with a closer contact interface and highly enhanced photocatalytic activity.

研究领域: 材料科学 · 化学工程 · 催化 · 纳米技术
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY · 2021 · IF 6.064

High-efficiency degradation of quinclorac via peroxymonosulfate activated by N-doped CoFe2O4/Fe0@CEDTA hybrid catalyst

Lezhu Su,Lizhou Ou,Yujiao Wen,Yifan Wang,Weilin Zhao,Zhi Zhou,Mei-e Zhong,Yongfa Zhu,Nan Zhou

Exploring catalyst materials which are advancing, recyclable and with high catalytic performances to remove persistent organic pollutants such as Quinclorac (QNC) is important. In this work, a novel N-doped carbon support CoFe 2 O 4 /Fe 0 hybrid catalyst (CFO/Fe@C) was in situ formed by a simple co-precipitation and calcination process. Fine intergrowth crystal CoFe 2 O 4 and Fe 0 were uniformly dispersed on the N-doped porous carbon that derived from the raw material Ethylene Diamine Tetraacetic Acid (EDTA), which also provided chelating effect to prevent the agglomeration of the metals. Interestingly, the Fe 0 could only be formed with the presence of cobalt, possibly due to the increased reduction property resulted from the particle refinement. The as-formed Fe 0 could not only activate the peroxymonosulfate (PMS) but also reduce the Co 3+ , resulting in a synergistic impact to remarkably enhance the degradation performance. Besides, the N-doped porous carbon can also benefit the degradation of pollutant by strengthening the electron transfer. A good degradation efficiency of QNC was obtained in CFO/Fe@C-PMS system and most of the QNC had been degraded to carbon dioxide , water and other small molecular organisms. The removal rate remained over 70% after four reuses and the material could be easily recovered from the solution due to the good magnetic properties. Therefore, the as-prepared CFO/Fe@C catalyst should be an ideal catalyst for the removal of organic pollutants .

研究领域: 环境科学 · 催化材料科学
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