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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.

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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2019 · IF 4.084

Multiporous core-shell structured MnO@N-Doped carbon towards high-performance lithium-ion batteries

Jing Lin,Lei Yu,Qujiang Sun,Fangkuo Wang,Yong Cheng,Sheng Wang,Xu Zhang

It is imminently to seek for high energy density in addition to a sensational lifetime of lithium-ion batteries (LIBs) to meet growing requisition in the energy storage application. Anode containing metal oxide composite is being thoroughly investigated for their higher capacity than that of the commercial graphite. A multiporous core-shell structured metal oxide composite anode possessing the excellent capacity and superb lifespan for LIBs is designed. In detail, metal oxide ( i.e., MnO) is encapsulated in N-doped carbon shell (MnO@N–C) via coprecipitation-annealing technique. During annealing, abundant void space among MnO cores/between MnO cores and N–C shells is obtained. This space can efficaciously buffer volume changes of MnO upon cycles. Benefiting from the unique structure and heteroatom doping , the capacity of MnO@N–C microcube anode exhibits 576 mAh g −1 at 5 A g −1 with an ultra-long lifespan more than 3500 cycles. The connection between the electrode characteristics and structure is concurrently examined by adopting kinetic analysis. Finally, a full lithium-ion battery is presented, applying the MnO@N–C (anode) and Nick-rich layered oxide (cathode). It is believed that structural designing with heteroatom doping can be utilized in vaster fields for superior capabilities.

✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2018 · IF 3.779

Controllable synthesis of N-C@LiFePO4 nanospheres as advanced cathode of lithium ion batteries

Q.Q. Xiong,J.J. Lou,X.J. Teng,X.X. Lu,S.Y. Liu,H.Z. Chi,Z.G. Ji

Exploring advanced cathode materials is critical for the development of large-scale lithium ion storage. Herein we report nitrogen-doped carbon (N-C) coated LiFePO 4 nanospheres (N-C@LFP) synthesized by a facile hydrothermal plus chemical polymerization method . N-C@LFP nanospsheres exhibit diameters of 400–700 nm and show core-shell structure with a thin N-C layer of ∼2.5 nm. As a cathode for lithium ion batteries (LIBs), N-C@LFP nanospheres present excellent electrochemical performance with higher electrochemical reactivity, better reversibility and smaller polarization as compared to the unmodified pristine LiFePO 4 nanospheres . The N-C@LFP electrode delivers superior specific capacity of 158.4 mAh g −1 after 200 cycles at 1 C and good rate capability (107.5 mAh g −1 at 30 C). The enhanced electrochemical performance is attributed to the conductive N-C layer coating with fast ion/electron transfer. The N-C@LFP nanospheres are thus promising for commercial application in high-energy & power LIBs.

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ENERGY & FUELS · 2014 · IF 2.733

Storage Capacity and Duration of Methane Hydration in a Slurry of Solid n-Tetradecane

Hongchao Yan,Xiaofei Song,Feng Xin,Xingang Li,Guangjin Chen,Yong Wang

Storage capacities, formation rates, and induction periods of methane hydrates in slurries of solid n-tetradecane, which is a phase change material (PCM), were investigated experimentally in a semibatch hydrator with a stirrer. The hydrations were carried out at an initial temperature of 277.1 K, which was slightly lower than the melting point of n-tetradecane in a slurry; the stirring rate was 800 rpm, and the experimental pressures were in the range of 5.00–6.28 MPa. The emulsion of PCM was prepared using a high-speed disperser and then cooled to solidify the PCM droplets in an oil-in-water (O/W) emulsion. The highest storage capacity of 158.7 V/V was found at 5.26 MPa, and the corresponding hydration time was only 78 min. The hydration rates divided into three stages: a constant speed was observed initially, followed by a steep increase, and a slowing in the final step. The maximum hydration rate was 0.0096 molCH4/(molH2O min) at 5.26 MPa. The induction time of hydration was reduced largely to a few minutes. Therefore, the fast formation rate and short induction time led to free water being trapped in the hydrate and much higher pressures would make the storage capacity smaller. Therefore, the advantage of our method is improving heat transfer during hydration, which results in a fast hydration rate and high storage capacity. On the other hand, one disadvantage is that the method is somewhat complex.

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Journal of Macromolecular Science Part A-Pure and Applied Chemistry · 2019 · IF 1.163

Poly(N-isopropylacrylamide)@graphene oxide-Ag responsive hydrogels. Characterization and smart tunable catalytic activity

Jing Chen,Qing Luo,Xiao Zhen Ma

Thermally responsive hydrogels have drawn significant research attention recently because of their simple use as smart catalyst. Here we design a series of responsive hydrogels that incorporate graphene oxide (GO)-Ag composites into thermo-responsive N-isopropylacrylamide (NIPAM) at different mass ratios. It was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric analysis (TGA), and UV-visible absorption spectroscopy. Meanwhile, the PNIPAM/GO-Ag hydrogels showed high catalytic activity in the hydrogenation reaction of nitrophenol to aminophenol and acted as a tunable catalyst which the swelling and collapsing could be triggered by small temperature changes around the lower critical solution temperature (LCST) of the hydrogels. The present approach can shed new light on designing of catalytic material like GO-Ag composite responsive hydrogel with promising applications in catalysis.

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RARE METALS · 2014 ·Vol. 33 ·期 1 ·86-90 · IF 0.806

Improving hydrogen storage performance of Li–Mg–N–H system by adding niobium hydride

Zhu Xi-Lin,Han Shu-Min,Zhao Xin,Li Yuan,Liu Bao-Zhong

Hydrogen storage properties of 2LiNH 2 –MgH 2 – x NbH ( x  = 0 and 0.05) composites and the catalysis of NbH on hydrogen sorption reaction of the Li–Mg–N–H system were investigated. Hydrogen sorption properties of 2LiNH 2 –MgH 2 system are effectively improved by adding NbH. Temperature programmed desorption results show the addition of NbH reduces the dehydriding onset temperature of 2LiNH 2 –MgH 2 system by 21 K. Approximate 3.62 wt% hydrogen in 2LiNH 2 –MgH 2 –0.05NbH composite is released following a 500 min at 433 K, whereas the amount of hydrogen desorption is only ~3.16 wt% for the pristine system under the same condition. The sample with NbH exhibits higher dehydriding rate compared with the pristine one. Moreover, hydrogen absorption rate increases by adding NbH into the 2LiNH 2 –MgH 2 system. Hydrogen absorption capacity of the samples with NbH is 3.23 wt% within 400 min, which is higher than that of pristine sample. Fine NbH particles homogeneously distribute in the 2LiNH 2 –MgH 2 –0.05NbH composite, and catalyze the hydrogen sorption reaction rather than reacts as a reactant into new compound.

✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 16 ·9665-9672 · IF 10.733

7.5% n–i–p Sb2Se3 solar cells with CuSCN as a hole-transport layer

Kanghua Li,Siyu Wang,Chao Chen,Rokas Kondrotas,Manchen Hu,Shuaicheng Lu,Chong Wang,Wei Chen,Jiang Tang

Sb2Se3 is a promising non-toxic, Earth-abundant, stable thin-film solar cell absorber material. However, the low built-in potential caused by the low intrinsic doping density (∼1013 cm−3) and the low carrier collection efficiency due to the low carrier mobility (∼1.5 cm2 V−1 s−1) hinder further efficiency improvement of Sb2Se3 solar cells. Therefore, an effective hole-transport layer (HTL) is necessary to further boost the built-in potential and assist carrier collection. Herein we attempt to improve the efficiency of Sb2Se3 solar cells by using CuSCN as an HTL. CuSCN as an HTL suppresses the back surface recombination, and enhances the built-in potential and carrier collection efficiency. Meanwhile, materials and physical properties characterization reveals that CuSCN provides Cu ions which induce grain boundary inversion, and therefore separate photo-generated carriers more efficiently. Consequently, we obtained a device efficiency of 7.50%.

✓ 已验证 DOI 高影响因子
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ACS Applied Energy Materials · 2021 · IF 6.024

Enhancement of Thermoelectric Properties in n-type NbCoSn Half-Heusler Compounds via Ta Alloying

Qin Wang,Jiamian Huang,Chenyang Wang,Pengfei Luo,Zhili Li,Rongtao Liu,Qunaying Ma,Jun Luo

NbCoSn-based half-Heusler alloys are promising n-type high-temperature thermoelectric materials, but their relatively high thermal conductivities prevent the further improvement in thermoelectric properties. In this work, an effective way to reduce the lattice thermal conductivity without degradation of electrical transport properties via the isoelectronic substitution of Ta for Nb in NbCoSn-based alloys has been demonstrated. The synthesis and thermoelectric properties of Nb1–xTaxCoSn0.9Sb0.1 (x = 0, 0.05, 0.1, 0.15, 0.2, and 0.25) solid solutions are reported. The large mass fluctuation and chemical bond softening caused by Ta alloying significantly suppress the lattice thermal conductivity. Meanwhile, the Ta content has little effect on the carrier mobility due to the close atomic size and similar chemical nature between Ta and Nb. Benefiting from the significant reduction of lattice thermal conductivity and preservation of electrical transport performance after Ta alloying, a ZT value of ∼0.7 is achieved in Nb0.75Ta0.25CoSn0.9Sb0.1 at 973 K, which is about 32% higher than that of a NbCoSn0.9Sb0.1 matrix. This work demonstrates a valid approach to enhance the thermoelectric performances of half-Heusler alloys.

✓ 已验证 DOI 高影响因子
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Energies · 2022 ·Vol. 15 ·期 8 ·2908 · IF 3.252

RuCo Alloy Nanoparticles Embedded into N-Doped Carbon for High Efficiency Hydrogen Evolution Electrocatalyst

Cheng Wang,Yibo Wang,Zhaoping Shi,Wenhua Luo,Junjie Ge,Wei Xing,Ge Sang,Changpeng Liu

For large-scale and sustainable water electrolysis, it is of great significance to develop cheap and efficient electrocatalysts that can replace platinum. Currently, it is difficult for most catalysts to combine high activity and stability. To solve this problem, we use cobalt to regulate the electronic structure of ruthenium to achieve high activity, and use carbon matrix to protect alloy nanoparticles to achieve high stability. Herein, based on the zeolitic imidazolate frameworks (ZIFs), a novel hybrid composed of RuCo alloy nano-particles and N-doped carbon was prepared via a facile pyrolysis-displacement-sintering strategy. Due to the unique porous structure and multi-component synergy, the optimal RuCo500@NC750 material in both acidic and alkaline media exhibited eminent HER catalytic activity. Notably, the 3-RuCo500@NC750 obtained a current density of 10 mA cm−2at 22 mV and 31 mV in 0.5 M H2SO4and 1.0 M KOH, respectively, comparable to that of the reference Pt/C catalyst. Furthermore, the Tafel slopes of the catalyst are 52 mV Dec−1and 47 mV Dec−1, respectively, under acid and alkali conditions, and the catalyst has good stability, indicating that it has broad application prospects in practical electrolytic systems. This work contributes to understanding the role of carbon-supported polymetallic alloy in the electrocatalytic hydrogen evolution process, and provides some inspiration for the development of a high efficiency hydrogen evolution catalyst.

✓ 已验证 DOI 高影响因子
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Nano Energy · 2018 · IF 13.12

Controllable tuning of Fe-N nanosheets by Co substitution for enhanced oxygen evolution reaction

Li An,Jianrui Feng,Yu Zhang,Yong-Qing Zhao,Rui Si,Gui-Chang Wang,Fangyi Cheng,Pinxian Xi,Shouheng Sun

Transition-metal nitrides (TMNs), especially iron-based TMNs, have high electrical conductivity , superior chemical stability and unique oxygen-reaction ability, and have emerged as a new form of noble metal-free electrocatalysts . In this paper, we demonstrate that the ORR-active/OER-inert single function catalyst Fe-N can be made as the OER/ORR-active bifunctional catalyst Co-Fe-N by controlled substitution of Fe with Co. To obtain atomic insights of the Co-enhanced OER catalysis, we develop a new exfoliation method to prepare atomically thin (1.1 nm) nanosheets (NSs) of Co x Fe 1-x N 0.5 (x = 0, 0.05, 0.1, 0.15 and 0.2). Our studies show that both electronic structure and local binding environment of Fe are modified by Co substitution and the Co-Fe-N NSs show a volcano−like OER catalysis with Co 0.15 Fe 0.85 N 0.5 NSs being the most efficient OER catalyst, showing the lowest overpotential of 266 mV at 10 mA cm −2 , a Tafel slope of ∼30 mV dec −1 , and excellent stability in the 1.0 M KOH OER condition. Density functional theory (DFT) calculations suggest that the Co-Fe sites in the Co 0.15 Fe 0.85 N 0.5 structure are optimized to promote OH* to O* conversion, O*-O* coupling and O 2 formation. The Co 0.15 Fe 0.85 N 0.5 NSs are a class of new noble-metal-free catalyst for OER.

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Materials Today Communications · 2021 · IF 3.383

Enhance Mg-based heat storage materials kinetics by complex oxides

Daifeng Wu,Rui Li,Tai Sun,Renheng Tang,Fangming Xiao

Mg/MgH 2 as a thermochemical energy storage (TCES) material suffers from a slow hydrogenation-dehydrogenation kinetic and poor reversibility. Addition of metal oxide is an effective way to improve the kinetic properties of Mg/MgH 2 . However, there is little study on the effects of complex oxides . Thus, the catalytic effects of complex metal oxides and its catalytic mechanism were investigated in this paper. Results show that the dehydrogenation peak temperature and apparent activation energy of MgH 2 -Ta 2 O 5 are 320.8 °C and 128.54 kJ/mol. Combined with complex metal oxide, MgH 2 -Ta 2 O 5 -Nd 2 O 3 could further reduce the dehydrogenation peak temperature (307.2 °C) and apparent activation energy (95.33 kJ/mol). MgO and NdH 2.61 are found in the dehydrogenated MgH 2 -Ta 2 O 5 -Nd 2 O 3 , indicating that n-typed oxide Ta 2 O 5 and p-typed oxide Nd 2 O 3 are formed and improved the kinetics properties of MgH 2 . Furthermore, Nd 2 O 3 /Ta 2 O 5 interface is formed and acted as “p-n junction”. When heating, the “p-n junction” is exposed to thermal radiation and produce electrons and holes, and then the kinetics properties of MgH 2 are further enhanced.

研究领域: 材料科学 · 能源化学 · 物理化学 · 无机功能材料 · 热能存储
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ANALYTICAL LETTERS · 2023 · IF 2

Novel Paper-Based Fluorescent Sensor Based on N-Doped Carbon Quantum Dots (N-CQDs) and Cotton Fiber Paper (CFP) with High Selectivity and Sensitivity for the Visual Determination of Mercury (II) in Environmental Waters

Shunwei Wu,Yongzheng Yin,Chunyan Sun,Chenghai Ma

A highly selective solid-state fluorescent sensor based on N-doped carbon quantum dots (N-CQDs) and cotton fiber paper (CFP) is reported for the determination of trace mercury (II)(Hg2+). The N-doped carbon quantum dots on cotton fiber paper (N-CQDs@CFP) was synthesized using a facile one-step microwave hydrothermal method. Multiple approaches were employed to fully investigate the morphology and chemical structure of the paper-based fluorescent sensor. The N-CQDs were chemically bonded onto the CFP, which offers good reproducibility and stability of the sensor. The N-CQDs@CFP showed high-intensity blue emission in dark-field imaging, and the fluorescence was quenched by Hg2+. The Hg2+ in aqueous samples was easily determined and visually monitored. There was good linearity from 0 to 250 μM, and the limit of detection was 34 nM. The paper-based fluorescent sensor provided accurate and rapid determination of Hg2+ upon comparison with flame atomic absorption spectrophotometry (FAAS). The simple preparation, rapid detection (< 5 min), low cost, and easy-handling illustrate that the reported sensor has a significant value in environmental monitoring.

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