SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Kuang Wang,Zhanqiang Fang
In this work, a cost-effective ball-milling technique was employed to synthesize submicron oxalated zero-valent iron co-doped with graphite and nickel (G@Fe OX bm /Ni), aiming to enhance the removal efficiency of the recalcitrant pollutant 2, 2′, 4, 4′ – tetrabromodiphenyl ether (BDE-47) while minimizing secondary risks. The incorporation of graphite significantly improved the debromination efficiency of BDE-47, with a rate constant of 0.26 day −1 in a tetrahydrofuran/water system, which represents a 59.88 % increase over the oxalated zerovalent Fe/Ni without graphite (0.16 day −1 ). The determination of Ni leaching showed that no nickel ions were detected post-reaction over a broad pH range (3–11). Moreover, the reactivity of G@Fe OX bm /Ni was largely unaffected across the pH range (0.26–0.49 day −1 ), exhibiting excellent resistance to acidic and alkaline conditions. In both ultrapure water and real groundwater matrices, the degradation rate constants for BDE-47 increased to 2.98 day −1 and 0.79 day −1 , respectively, achieving debromination yields of 97.86 % and 50.18 % for the final product, diphenyl ether. Based on the established degradation pathway and electrochemical analysis, the debromination of BDE-47 follows a catalytic debromination and hydrogenation process by adsorbed atomic hydrogen (H* ADS ). The graphite doping enhanced the debromination of BDE-47 by increasing the production of H* ADS . The adsorption effect of graphite on metal ions effectively controlled secondary pollution and improved the material’s tolerance to acidic and alkaline environments. This work offers an efficient method for the degradation of low brominated diphenyl ether pollutants at a low cost and without secondary risks.
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ENVIRONMENTAL POLLUTION
·
2024
·
IF 7.6
Kuang Wang,Zhanqiang Fang
In the homologous series of polybrominated diphenyl ethers (PBDEs), the debromination of low-brominated diphenyl ethers with higher toxicity remains a challenge. Nano zero-valent iron (nZVI) has been extensively studied for the debromination of PBDEs, but its inherent direct electron transfer mechanism is less efficient for low-brominated diphenyl ethers, and there are issues with high preparation costs. In this work, we synthesize Ni-doped oxalated submicron ZVI (Fe OX bm /Ni) using a low-cost ball-milling method. Fe OX bm /Ni exhibits a debromination rate constant of 0.48 day −1 for 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) in tetrahydrofuran (THF)/water. The debromination rate of Fe OX bm /Ni for BDE-47 in water is even faster (0.98 day −1 ), with the yield of the complete debromination product, diphenyl ether, reaching 76.71%. In real groundwater, Fe OX bm /Ni also shows high reactivity toward BDE-47, with a rate constant of 0.33 day −1 . Kinetic experiments, quenching experiments, and degradation pathway indicate that the attack of atomic hydrogen on C-Br bonds is the primary degradation mechanism. Electrochemical analysis further show that Ni 0 sites could cleave hydrogen into absorbed atomic hydrogen (H∗ ABS ) and adsorbed atomic hydrogen (H∗ ADS ), with H∗ ADS playing the main role. These findings contribute valuable insights into advancing the large-scale application of ZVI and offer promising strategies for thorough remediation of PBDEs pollution.
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Wangli Yao,Tian Liu,Jingxian Zheng,Saitao Yan,Baoliang Chen,Xiaoying Zhu
Conventional catalytic membranes often exhibit inadequate catalytic efficiency due to limited retention time for pollutants during filtration. In this study, a single-atom catalyst (Ni-NG) was prepared by dispersing single nickel atoms onto nitrogen-doped graphene oxide sheets. Subsequently, under controlled conditions, the assembly of Ni-NG with reduced graphene oxide (rGO) sheets led to the fabrication of efficient electrocatalytic cathodic membranes (ECMs). The ECMs were designed to concentrate and dehalogenate antibiotics simultaneously by utilizing the confined single nickel atoms within the multilayered ECMs through electrocatalytic reduction. Remarkably, complete degradation of chloramphenicol (CAP, 20 mg L −1 ) in the solution was achieved within a remarkably short time of 3.0 ms by ECM8 which had an area of 7.1 cm 2 and comprised Ni-NG (16.9 μg) and rGO (16.9 μg), with an interlayer spacing of 0.37 nm, during filtration (40 L m −2 h −1 ). The reaction rate constant (k) for CAP degradation by ECM8 was approximately 3 × 10 8 min −1 , surpassing the highest value in the literature. Furthermore, the ECM demonstrated both high energy efficiency and stability, highlighting the great potential for practical applications. The electrocatalytic cathodic membrane, designed to primarily concentrate pollutants in confined interlayer spaces through the sieving effect, shed lights on the highly efficient dehalogenation of organic compounds in pharmaceutical salt-laden wastewater.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Jiaxing Song,Jiabao lv,Yuhan Pan,Jingyu Wang,Jun Wang,Ang Cao,Angjian Wu,Paul T. Williams,Qunxing Huang
Conventional catalytic pyrolysis of waste plastics for H 2 production faces challenges due to excessively high reaction temperatures. This study introduced a NiCeOx/β catalyst for low-temperature H 2 production from polyethylene (PE), aiming to enhance H 2 yield through nonthermal plasma (NTP) and catalytic active sites. Experimental results confirmed the efficacy of NTP in promoting collision between high-potential-energies active species and plasma-catalyst interactions, identifying acidic sites as primary catalytic active sites. Both experiments and density functional theory (DFT) calculations confirmed NiO and CeO 2 particles as metallic active sites, exhibiting thermodynamic and kinetic benefits for primary products from PE pyrolysis. Under optimal conditions, the highest H 2 yield and selectivity respectively reached 32.71 mmol/g and 82.10 % at a PE/(NiCeOx/β) ratio of 1:4, reaction temperature of 400 °C, and NTP discharge power of 210 W. The NiCeOx/β catalyst facilitated low-temperature pyrolysis of waste plastics, enhancing H 2 selectivity and yield.
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Small
·
2024
·
IF 13
Zhipeng Liu,Jinling Xue,Yibin Fan,Yinshi Li
Rational design of efficient and non-noble metal bifunctional catalysts for alkaline overall water splitting (OWS) electrochemical reactions is of top priority in the development of hydrogen-based energy. Constructing catalysts with unique structures to optimize the intrinsic activity is a promising strategy. In this work, a newly developed Ni 3 Co 3 Mo 100 -BTC-15h catalyst consisting of Ni nanoparticles enriched on the surface along with a core-shell porous structure is prepared via a hydrothermal process. Due to the unique composition and Ni-enriched core–shell structure, the Ni 3 Co 3 Mo 100 -BTC-15h catalyst exhibits enhanced electrocatalytic properties for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in alkaline media. Under the dual tuning and intermetallic phase, the Ni 3 Co 3 Mo 100 -BTC-15h catalyst deliver a lower overpotential of 151 mV and ≈ 136 mV exceeding commercial catalysts for OER and HER. When the Ni 3 Co 3 Mo 100 -BTC-15h is used as bifunctional catalyst for OWS in a two-electrode alkaline electrolyzer, a cell voltage of 1.62 V is required to drive 10 mA·cm −2 comparable to that of commercial Pt/C and RuO 2 catalysts. This work proposes a potential strategy for optimizing the electrocatalytic performance of non-noble metal catalysts for OWS.
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Matter
·
2025
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IF 17.5
Shining Wu,Yuting Zhang,Guanwu Li,Yifeng Hou,Mengyang Cao,Chengyu Wei,Pengkun Yang,Lu Huang,Yingpeng Wu
High-entropy alloys (HEAs) have a wide range of applications due to their excellent physical and chemical properties. However, traditional synthesis routes always require high temperatures over 923 K or have high equipment requirements. Here, we developed a liquid metal gallium (Ga)-mediated strategy using only a commercial vortex mixer and metal powders to synthesize HEAs near room temperature (303 K) with low power (7 W). A variety of HEAs were successfully prepared, and the yield can be expanded to over 10 g each time. The mechanistic investigation proved that Ga continued to flow under the mechanical force and exposed fresh surfaces to contact the metal, thereby promoting the process of metal dissolution in Ga and forming HEAs. These as-prepared HEAs can be used for catalysis in electrochemical oxygen evolution reactions with low overpotential and high durability. This strategy provides an innovative method for low-energy synthesis of HEAs at room temperature.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Qingming Zeng,Yanjun Wen,Xiaoguang Duan,Xing Xu,Jing Tan,Qingyan Zhang,Yilin Liu,Qingyi Zeng
In this work, we revealed a dual-pathway nonradical oxidation (NRO) system catalyzed by Ni single atom catalyst (NiN 4 ) accommodated in the carbon nitride substrate. The monatomic Ni coordinated with four N atoms (Ni-N 4 ) is determined as the dynamic catalytic center for peroxymonosulfate (PMS) activation, showing an exceptional specific rate constant of 3.34 min −1 g −2 L −2 (29.7 times that of CN/PMS system) in oxidizing bisphenol A and other refractory organics. In situ Raman, X-ray absorption, and electrochemical analyses as well as theoretical simulations demonstrate that the Ni-N 4 sites exhibit strong interaction with PMS benefited from the modulated electronic structures, resulting in nonradical surface-bonding active complexes (NiN 4 -PMS*) and deuterogenic high-valent Ni(IV)-Oxo species. The dual-pathway NRO process will spontaneously coordinate both electron transfer process via CN matrix and direct electron transfer by Ni(IV)-Oxo for selective organic oxidation with excellent anti-interference ability and adaptability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yanling Wang,Yu Wang,Wensheng Fu,Guanyun Gao,Yanru Liu,Lei Wang
The preparation of low-cost and high-activated catalysts is an important challenge in the development of hydrogen production industry. Here we reported a novel core-shell triangular cone electrocatalyst Ni 3 S 2 @Ni 3 N@Co 2 N 0.67 grown on nickel foam (Ni 3 S 2 @NiCoN/NF) obtained by a self-templated method. The obtained Ni 3 S 2 @NiCoN/NF consists of Ni 3 S 2 triangular cone core and Ni 3 N@Co 2 N 0.67 particles shell, which has rich heterogeneous interface and synergistic effect. The strong electronic interaction at the newly bonded heterojunction regulates the electronic structure of active Ni, which is conducive to the transfer of charge to the active site. In addition, NiCoN particles are coated on the surface of Ni 3 S 2 triangular pyramidal nucleus to form a core-shell structure, which can make sure the exposure of active sites. It is found that the self-templated conversion of Co(OH) 2 coated Ni 3 S 2 into NiCoN/Ni 3 S 2 enhances the activity for hydrogen evolution reaction (HER). The hybrid material has excellent HER catalytic performance under alkaline conditions, which only needs to overcome the overpotential of 63 and 174 mV to reach the current density of 10 and 100 mA cm −2 , respectively. This study provides a new idea for the preparation of efficient and stable catalysts with core-shell structure for HER.
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ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Mingchen Xu,Xinfa Zhu,Gaoning Fan,Xiyu Jia,Yonghui Zhang,Mengjun Wang,Hongxing Zheng,Pengyu Zhou,Chao Fan
Visible photodetectors based on two-dimensional tin disulfide (SnS2) have attracted interest for applications in optical communication, information capture, and military reconnaissance owing to their high absorption efficiency, atomic-scale thickness, and nontoxicity. However, their intrinsic bandgap limits their spectral detection range, hindering further practical applications. Herein, we introduce VIII B-nickel (Ni) with a similar ionic radius to Sn to form Ni-doped SnS2 few-layers via micromechanical exfoliation. As the Ni-doping concentration increases, the bandgap decreases from 2.14 (SnS2) to 1.95 eV (Sn0.9Ni0.1S2). Subsequently, Ni-doped SnS2-based photodetectors are fabricated and characterized. These devices exhibit an extended spectral detection range and excellent performance, with a maximum responsivity of 2009 A W–1 and high normalized detectivity of 2.47 × 1012 cm Hz1/2 W–1. Furthermore, to suppress dark current and noise, SnS2/Ni-doped SnS2 homostructures and their corresponding photodetectors are fabricated. The built-in electrical field of the homostructure effectively reduces the dark current of the homostructure photodetector to 110 nA. Consequently, the responsivity is enhanced to 3350 A W–1 and the response time is reduced to 3.5 ms, outperforming most other 2D material–based and commercial photodetectors. And Ni-SnS2 VPDs show an application potential in imaging and visible-light communication systems. Thus, this study presents an effective approach to extend the detection spectrum of SnS2-based photodetectors and pave the way for their future applications.
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MOLECULES
·
2024
·Vol. 29
·期 9
·2092
·
IF 4.2
Zhi Lu,Shilin Li,Laiyuan Ning,Kun Tang,Yifan Guo,Long You,Chong Chen,Guangxin Wang
Developing high-performance and cost-competitive electrocatalysts have great significance for the massive commercial production of water-splitting hydrogen. Ni-based electrocatalysts display tremendous potential for electrocatalytic water splitting. Herein, we synthesize a novel NiFe-layered double hydroxide (LDH) electrocatalyst in nanosheets array on high-purity Ni foam. By adjusting the Ni/Fe ratio, the microstructure, and even the behavior of the electrocatalyst in the oxygen evolution reaction (OER), changes significantly. The as-obtained material shows a small overpotential of 223 mV at 10 mAcm−2as well as a low Tafel slope of 48.9 mV·dec−1in the 1 M KOH electrolyte. In addition, it can deliver good stability for at least 24 h of continuous working at 10 mAcm−2. This work proposes a strategy for engineering catalysts and provides a method for the development of other Ni-based catalysts with excellent performance.
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MOLECULES
·
2024
·Vol. 29
·期 16
·3966
·
IF 4.2
Zhi Lu,Shilin Li,Yuxin Wang,Jiefeng Wang,Yifan Guo,Jiaqi Ding,Kun Tang,Yingzi Ren,Long You,Hongbo Meng,Guangxin Wang
Water splitting is an important approach to hydrogen production. But the efficiency of the process is always controlled by the oxygen evolution reaction process. In this study, a three-dimensional nickel–molybdenum binary nanoarray microstructure electrocatalyst is successfully synthesized. It is grown uniformly on Ni foam using a hydrothermal method. Attributed to their unique nanostructure and controllable nature, the Ni-Mo-based nanoarray samples show superior reactivity and durability in oxygen evolution reactions. The series of Ni-Mo-based electrocatalysts presents a competitive overpotential of 296 mV at 10 mA·cm−2for an OER in 1.0 M KOH, corresponding with a low Tafel slope of 121 mV dec−1. The three-dimensional nanostructure has a large double-layer capacitance and plenty of channels for ion transfer, which demonstrates more active sites and improved charge transmission. This study provides a valuable reference for the development of non-precious catalysts for water splitting.
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Journal of Energy Storage
·
2024
·
IF 8.9
Chongjun Zhao,Haimin Ou,Chunhua Zhao
Energy storage devices serve critical roles in both harvesting energy from new energy sources and supplying energy to consumers, and the performance of supercapacitors is heavily reliant on the performance of activated material, which is determined by the qualities achieved during the specified preparation process. Herein, due to the merit of isotropy of 0D carbon nanoparticles in structure and current transfer, spherical carbon aerogels (CA) with the size of ϕ ~ 100 nm are carbonized within 3 min in air in an open tube furnace, in which those waste epoxy resin blocks are chosen and reused as the carbon source. After the activation, the surface of activated CA (ACA) becomes rough, and its specific surface area reaches 1222.40 m 2 ·g −1 . The above ACA owns high electrochemical supercapacitor performance: Referring to the ACA-based electrode, a specific capacitance of 298.8 F·g −1 at 1 A·g −1 and 92.81 % retention after 20,000 cycles of repeated charge/discharge. As for its symmetric supercapacitor (SSC), it has good CV behavior even at 1000 mV·s −1 , accompanied by an energy density of 20.92 W h·kg −1 at the power density of 300 W·kg −1 , and 12.34 W h·kg −1 even at 12000 W·kg −1 .
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