SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Linzhi Shen,Ziwen Xiong,Zhaohui Du,Hao Wang,Wenrui Li,Zhen Zhang,Hao Wu,Changsong Zhou,Yaming Zhou,Guanghua Tang,Jing Liu,Hongmin Yang
M-N-C catalysts have considerable potential in the fields of catalysis, such as highly polluting gaseous elemental mercury (Hg 0 ) oxidation. However, the direct application of these kinds of catalysts for mercury removal is stymied by their low catalytic efficiency. Heteroatom-doping in M-N-C catalysts has been proposed as a powerful strategy to the promote catalytic of Hg 0 , but the origin of boosting catalytic activity is still elusive. Herein, it is disclosed that selenium doping induces an obvious electron-acceptor effect for accelerating the Hg 0 catalytic oxidation. The model selenium-doped Cu-N-C catalyst with atomically dispersed active sites was verified by various characterization methods, such as SEM-EDS and scanning transmission electron microscopy. The optimal Cu-NC-Se with Cu/Se ratio of 1:1 exhibited the best Hg 0 removal performance, over 8-fold enhancement in their Hg 0 oxidation capacities than raw selenium-free Cu-NC. At the optimal reaction temperature of 90 °C, Cu-NC-Se achieved an average Hg 0 removal rate of 92.44% within 60 min under single pure N 2 atmosphere. As for the influence of flue gas components, the presence of O 2 promoted the removal of mercury in Cu-NC-Se, whereas CO 2 , NO and SO 2 served as slight inhibitors. Even after five cycles of the experiment, the average mercury oxidization efficiency was still remained at 88.5%, showing that Cu-NC-Se can be reused with good maintenance of the catalytic activity and atomic dispersion of Cu and Se in the structure. The unsaturated Cu sites connected with pyridinic N on the carbon matrix can serve preferential adsorption to Hg 0 and doped selenium. Meanwhile, the selenium doping accelerated Hg 0 adsorption and accept sufficient electrons for promoting Hg 0 oxidation to forming stable HgSe, which is also corroborated by the theoretical analysis results based on density functional theory. This work not only provides an alternative facile synthetic strategy for developing heteroatom-doping atomically dispersed M-N-C catalysts, but also represents a significant advance for deepening the understanding of the Hg 0 catalytic oxidation mechanism on M-N-C catalyst.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Yihua Cao,Zhi Li,Xueli Yin,Yonghao Gan,Ying Ye,Run Cai,Qi Wang,Bo Feng,Xiaoping Dai,Weiyu Song
The development of low-cost and high-efficiency electrocatalysts for the oxygen evolution reaction (OER) is essential to produce high-purity hydrogen in large scale. Herein, a three-dimensional (3D) seaweed-like hierarchical structure was fabricated using two-dimensional (2D) NiMn LDH nanosheets wrapped on one-dimensional (1D) NiSe nanowires with nickel foam (NF) as a substrate (NiSe@NiMn LDH/NF) via hydrothermal and electrodeposition processes. Owing to the strong interfacial synergy, 3D seaweed-like hierarchical structure, higher conductivity, and strong structural stability, the NiSe@NiMn LDH/NF exhibited superior OER performance with an overpotential of 287 mV at 100 mA cm −2 , and stably operated for 160 h at large current. Moreover, the overall water splitting system with NiSe@NiMn LDH/NF as the anode and Pt/C/NF as the cathode exhibited a low cell voltage of 1.59/1.64 V to reach 50/100 mA cm −2 , and excellent stability for 110 h at 300 mA cm −2 . The density function theory (DFT) calculations unveiled that NiSe@NiMn LDH enabled the interfacial synergy, reallocating the electron density at the interface, and further weakening the energy barrier of OH* by strengthening chemical bonds with OH* intermediates to improve the intrinsic OER activity.
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PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
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2023
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IF 2.7
Jiapeng Zhang,Hui Zhang,Qinghua Du,Xinjian Xie,Yi Fang,Chengchun Tang,Guifeng Chen
Quantum dots (QDs) of I-III-VI 2 ternary compounds, such as CuInSe 2 (CISe) and CuInS 2 (CIS), have broad application prospects as light-absorbing layers in solar cells due to their excellent photoelectric properties. Nevertheless, the presence of large numbers of surface defects in quantum dots will affect their performance. In this study, inverted type-I CdS/CISe core-shell QDs are successfully synthesized through thermal injection method in triethylene glycol, which is green and safe. By changing the molar ratios of CdS and CISe QDs, the components and optical properties of core-shell QDs are intensively studied by using different characterization methods (XRD, TEM, EDS, UV–vis, Raman, and fluorescence spectrum). The solar cells with the structure of FTO/TiO 2 /CdS/CdS/CISe/Mo are assembled, where the CdS/CISe core-shell QDs are used as absorption layers. The prepared devices exhibit an efficiency of 1.01% under an AM 1.5 G spectrum with a light intensity of 100 mW cm −2 .
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Minghao Bao,Junhong Chen,Bozhong Pi,Qizhen Zhang,Zhongbo Han,Hongbiao Huo,Chunpei Yu,Wenchao Zhang
A green electrocatalytic system for co-production of SATz energetic material and H 2 . • Clean electrons replace hazardous chemical oxidants for SATz synthesis with SATz yield of 75.2%. • CoSe 2 @MoSe 2 @Pt/NF achieves 30 mV@10 mA·cm −2 and 192 mV@10 mA·cm −2 overpotential for HER. • Coupling system achieves low cell voltage of 1.44 V at 10 mA·cm −2 . Replacing the kinetically sluggish oxygen evolution reaction (OER) with thermodynamically more favorable electrochemical oxidation reactions represents an effective strategy to enhance energy efficiency and economic viability in water electrolysis. Herein, we designed a CoSe 2 @MoSe 2 @Pt/NF heterostructured catalytic electrode and construct an integrated electrocatalytic coupling system that enables the co-production of azo-bridged nitrogen-rich energetic material (sodium 5,5′-azotetrazolate, SATz) at the anode and clean hydrogen energy at the cathode. Mechanistic studies reveal that hydroxyl radicals generated via water electrolysis initiate the oxidative coupling of 5-aminotetrazole, achieving a SATz yield of 75.2% under optimized conditions. The CoSe 2 @MoSe 2 @Pt/NF cathode exhibits exceptional HER catalytic activity with a low overpotential of 192 mV at 100 mA·cm −2 and a Tafel slope of 50.2 mV·dec −1 , along with remarkable stability. Notably, the assembled coupling system requires a substantially reduced cell voltage of only 1.44 V to achieve 10 mA·cm −2 , significantly lower than that of conventional overall water splitting (>1.71 V). This work presents a sustainable and energy-efficient strategy for the simultaneous production of green energetic materials and clean hydrogen fuel, opening new avenues for advanced electrocatalytic coupling systems. Download: Download high-res image (166KB) Download: Download full-size image
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Ling Wang,Changzheng Lin,Miaoling Hu,Wei Yan
Due to the high theoretical capacity, metal selenides are considered to be promising materials for energy storage. Unfortunately, their practical use is still hampered by their flat electronic conductivity, large volume change and poor ion transport kinetics. In this work, a general synthesis method is presented for the preparation of metal selenides embedded in N-doped carbon nanofibers with in-situ grown carbon nanotubes (CNTs) on the surface (MSe 2 @NCF/CNTs, M=Co, Ni, Fe) as binder-free anodes for sodium-ion batteries. Metal precursors can be used as catalysts and as active materials after selenization treatment. The metal selenides are dispersed in the carbon nanofibers and CNTs, which effectively prevents agglomeration of the particles. The in-situ grown CNTs are strongly coupled to the surface of nanofibers, which improves the electrical conductivity , allows for efficient electrolyte infiltration and buffers the volume expansion during the charge/discharge processes. As a result, CoSe 2 @NCF/CNTs achieves extremely high reversible capacity, stable cycling stability (441.2 mAh g −1 after 1000 cycles at 200 mA g −1 ), and excellent rate properties (375.4 mAh g −1 at 2 A g −1 ) when used as binder-free anodes for sodium-ion batteries. The fast charge transport and Na + diffusion rates, as well as a pseudocapacitance Na + storage mechanism, are revealed by kinetic analysis. This synthetic approach is extendable to assembling CNTs in-situ on other substrates for advanced energy storage systems.
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Nano-Micro Letters
·
2023
·Vol. 16
·期 1
·1-21
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IF 26.6
Zhao Tianbao,Jia Zirui,Liu Jinkun,Zhang Yan,Wu Guanglei,Yin Pengfei
Electromagnetic wave (EMW) absorbing materials have an irreplaceable position in the field of military stealth as well as in the field of electromagnetic pollution control. And in order to cope with the complex electromagnetic environment, the design of multifunctional and multiband high efficiency EMW absorbers remains a tremendous challenge. In this work, we designed a three-dimensional porous structure via the salt melt synthesis strategy to optimize the impedance matching of the absorber. Also, through interfacial engineering, a molybdenum carbide transition layer was introduced between the molybdenum selenide nanoparticles and the three-dimensional porous carbon matrix to improve the absorption behavior of the absorber. The analysis indicates that the number and components of the heterogeneous interfaces have a significant impact on the EMW absorption performance of the absorber due to mechanisms such as interfacial polarization and conduction loss introduced by interfacial engineering. Wherein, the prepared MoSe 2 /MoC/PNC composites showed excellent EMW absorption performance in C , X , and K u bands, especially exhibiting a reflection loss of − 59.09 dB and an effective absorption bandwidth of 6.96 GHz at 1.9 mm. The coordination between structure and components endows the absorber with strong absorption, broad bandwidth, thin thickness, and multi-frequency absorption characteristics. Remarkably, it can effectively reinforce the marine anticorrosion property of the epoxy resin coating on Q235 steel substrate. This study contributes to a deeper understanding of the relationship between interfacial engineering and the performance of EMW absorbers, and provides a reference for the design of multifunctional, multiband EMW absorption materials.
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Small
·
2023
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IF 13.3
Jinchang Xu,Jiaxi Ruan,Yongqi Jian,Jiayu Lao,Zilong Li,Fangyan Xie,Yanshuo Jin,Xiang Yu,Ming-Hsien Lee,Zhenyou Wang,Nan Wang,Hui Meng
To overcome the low efficiency of overall water splitting, highly effective and stable catalysts are in urgent need, especially for the anode oxygen evolution reaction (OER). In this case, nickel selenides appear as good candidates to catalyze OER and other substitutable anodic reactions due to their high electronic conductivity and easily tunable electronic structure to meet the optimized adsorption ability. Herein, an interesting phase transition from the hexagonal phase of NiSe (H-NiSe) to the rhombohedral phase of NiSe (R-NiSe) induced by the doping of cobalt atoms is reported. The five-coordinated R-NiSe is found to grow adjacent to the six-coordinated H-NiSe, resulting in the formation of the H-NiSe/R-NiSe heterostructure. Further characterizations and calculations prove the reduced splitting energy for R-NiSe and thus the less occupancy in the t 2g orbits, which can facilitate the electron transfer process. As a result, the Co 2 -NiSe/NF shows a satisfying catalytic performance toward OER, hydrogen evolution reaction, and (hybrid) overall water splitting. This work proves that trace amounts of Co doping can induce the phase transition from H-NiSe to R-NiSe. The formation of less-coordinated species can reduce the t 2g occupancy and thus enhance the catalytic performance, which might guide rational material design.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jingwei Liang,Shaobin Li,Fengbo Li,Li Zhang,Yufeng Jiang,Huiyuan Ma,Kun Cheng,Liang Qing
The pursuit of cost-effective catalysts for electrocatalytic overall water splitting continues to present a significant challenge in the field. A molybdenum (Mo)-regulated Co 9 Se 8 /FeNiSe self-supporting electrode material with rich vacancy defects has been prepared by hydrothermal reaction. Doping of Mo atoms not only can form rich selenium vacancy defects to enrich the inherent activity of the catalyst, but also expose more active sites. The intrinsic electronic architecture of the interface catalysis is regulated and optimized through the introduction of heteroatom Mo, resulting in the exceptional catalytic activities of the Mo-Co 9 Se 8 /FeNiSe heterostructure. Additionally, the Faraday efficiency of hydrogen (H 2 ) and oxygen (O 2 ) production approaches 100 %. The voltage required for the water-splitting system is only 1.58 V (10 mA cm −2 ), and 100 h stability test at 100 mA cm −2 demonstrates no decay. This work presents a new perspective for the reasonable design and synthesis of non-precious metal selenide-based bifunctional electrocatalysts.
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ACS Applied Electronic Materials
·
2023
·
IF 4.7
Jingtao Li,Yang Ma,Xiaoting Wang,Wenling Li,Jingjie Li,Mengchen Zhou,Hu Chen,Wei Gong,Yongzhe Zhang
To take full use of the outstanding photoelectric properties of two-dimensional transition-metal dichalcogenides (2D TMDs), techniques for tuning their band gaps have been developed, among which defect engineering is found to be an effective way for broadband spectrum photodetection. Methods like pulsed laser deposition, thermal annealing, electron/proton beam etching, etc., can effectively reduce band gaps by introducing vacancy defects into TMDs, but they face the problems of high costs, uneven distribution of prepared defects, and unstable material properties. To solve these problems, we proposed a two-step strategy from “alloy synthesis” to “vacancy introduction”. Taking use of the bond energy differences between W–Se and W–Te in ternary alloy, WSe2(1–x)Te2x samples with homogeneous distributions of Se and Te were first synthesized, and then vacancy defects could be introduced through controllable release of Te atoms during a hydrogen-assisted annealing process, resulting in ∼4.1% vacancy defects with uniform distribution. A 910 nm photoluminescence (PL) peak appears in the annealed WSe2(1–x)Te2x, exhibiting a 110 nm red shift from the 800 nm peak of the unannealed alloy. Photoresponse of up to 1000 nm of the corresponding device verifies that a broadband spectrum detection TMD device has been successfully achieved in this study.
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Batteries & Supercaps
·
2023
·
IF 5.7
Weiquan Liang,Mingjie Liu,Xiaoyan Shi,Bin Chen,Lianyi Shao,Junling Xu,Zhipeng Sun
Graphical A solvent-free method was used to realize the efficient component regulation of target multivariate MOFs/MXene-derived multi-metal selenides@C/MXene (NCMS@C/MX) composites. The electrochemical performance of these composites can be optimized due to the intrinsic characteristics of the containing metal selenides. Metal-organic frameworks (MOFs) are excellent precursors for electrode materials preparations. Synergistic effects may exist between different metal centers in multivariate MOFs, making them often more effective than single-metal MOFs. Herein, we propose an atom economic mechanochemical method to realize the efficient component regulation of target multivariate MOFs. Moreover, by combining the synthesis of multivariate MOFs and exfoliating MXene, multivariate MOF/MXene composites can be obtained via a one-step strategy. A further selenization process can derive them into selenides@C/MXene composites. These derived composites contain multiple nanostructured metal selenides embedded in multi-heteroatom doped carbon matrix. For these composites, abundant heterojunction structures are formed, which can build internal self-built electric field and enhance the reaction kinetics effectively for sodium-ion storage. More importantly, the electrochemical performance of NCMS@C/MX composites can be optimized due to the intrinsic characteristics of the containing metal selenides. Overall, experimental results demonstrate the universality of this solvent-free synthesis route for controllable preparation of high-performance selenides@C/MXene electrode materials. It provides a feasible and environmentally friendly method to adjust metal ratios for optimal energy storage performance. We hope this research inspires optimization strategies for high-performance electrode materials and leads to the development of energy storage materials with more rational structures and better performance.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Dongmin Zhao,Zhuoyan Li,Kaini Zhu,Ai Lu,Ying Wang,Jingjing Jiang,Cong Tang,Xing-Can Shen,Changping Ruan
Owing to the strong Hg−Se interaction, Se-containing materials are promising for the uptake and immobilization of Hg(II) ions; compared with metal selenides or selenized compounds, elemental Se contains the highest ratio of Se. However, it remains a challenge to fully expose all the potential Se binding sites and achieve high utilization efficiency of elemental Se. Through rational design on the structure, dispersity, and size of materials, Se/CNF aerogels composed of abundant well-dispersed and amorphous nano-Se have been prepared and applied for the high-efficient uptake and immobilization of Hg(II) ions. The well-dispersion of nano-Se increases the exposure of Se sites, the amorphous structure benefits the easy cleavage of Se−Se bonds, the 3D porous networks of aerogels permit fast ions transport and easy operation. Benefiting from the combination effect of strong Hg−Se interaction and sufficient exposure of Se-enriched sites, the Se/CNF aerogels demonstrate strong binding ability ( K d = 3.8 ×10 5 mL·g -1 ), high capacity (943.4 mg·g -1 ), and preeminent selectivity ( α M Hg > 100) towards highly toxic Hg(II) ions. Notably, the utilization efficiency of Se in Se/CNF aerogels is as high as 99.5%. Moreover, the strong Hg−Se interaction and extraordinary stability of HgSe could minimize the environmental impact of the spent Se/CNF adsorbents after its disposal.
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ChemistrySelect
·
2023
·Vol. 8
·期 45
·e202302698
·
IF 2.1
Huiyan Wu,Zhaowei Liang,Zihan Zhang,Naijia Jiang,Jianhua Luo,Liyun Yang,Zhiqiang Zhou
Graphical An “on-off-on” nanoprobe for detecting Cd 2+ was developed using CdSe QDs. Based on the formation of CdSe/CdS QDs, Cd 2+ could restore the fluorescence of CdSe QDs quenched by S 2− . The fluorescence increased with increasing concentration of Cd 2+ in the range of 0.2–9 μM with low detection limit of 27 nM. In this work, an “on-off-on” nanoprobe for specific detection of Cd 2+ was constructed using N -acetyl- l -cysteine (NAC)-modified CdSe quantum dots (QDs). The prepared CdSe QDs exhibit characteristic green fluorescence. The adsorbed S 2− on the surface of CdSe QDs leads to dangling bonds and causes the fluorescence quenching of QDs, where the fluorescence of the system turns “off“. When Cd 2+ exists, it can react with the adsorbed S 2− to form CdS shell, resulting in the fluorescence enhancement of CdSe QDs, where the fluorescence of the system turns “on”. Due to the similar lattice structure between CdSe and CdS, CdSe/CdS can be produced by shell deposition, while self-nucleation of metal sulfide is observed in the presence of other metal ions. Thus, the developed nanoprobe shows high selectivity for Cd 2+ . Under the optimum sensing conditions, the fluorescence sensing signal of CdSe QDs depends linearly on the Cd 2+ in the range of 0.2–9 μM. The limit of detection (LOD) and limit of quantification (LOQ) of this nanoprobe is 27 nM and 90 nM, respectively. Furthermore, the proposed nanoprobe can monitor Cd 2+ in drinking water with a recovery rate between 95.82 % and 102.00 %, indicating its good practicability and applicability for real sample analysis.
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