APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yang Liu,Yuanpeng Huang,Xiangfang Peng,Chenglu Liang
Oxygen evolution reaction (OER) with four-electron process is the bottleneck of water electrolysis to produce hydrogen. In this work, selective surface nitridation of the self-supported Co oxide nanobushes was conducted to form the Co 5.47 N@Co oxide nanobushes catalyst electrode for OER. During the surface thermo nitridation, the N atoms replaced the sites of O atoms, causing lattice expansion/distortion along with rich oxygen vacancies. Besides, the nitridation promoted the charge transfer on the catalysts surface. As a result, the electronic states of the Co centers were modified and their catalytic activities towards OER were optimized. Combined with the DFT calculations and the experimental results, it was suggested that compared with the Co oxide nanobushes, the intermediates evolution during OER process was more spontaneous in the Co 5.47 N@Co oxide nanobushes electrode and their charge transfer resistance was greatly reduced, which displayed excellent OER performances in alkaline electrolyte, with the overpotentials of 208/287 mV at the current densities of 10/100 mA cm −2 and stabilized at the high current density of 100 mA cm −2 for over 20 h.
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ChemSusChem
·
2023
·Vol. 16
·期 10
·e202202078
·
IF 8.4
Weixia Huang,Yun Tong,Dongmei Feng,Zhendong Guo,Runze Ye,Pengzuo Chen
Graphical A novel self-supported Co 3 N nanowire arrays with Mo doping is designed by the hydrothermal and nitridation processes, serving as excellent electrocatalysts for overall water splitting. The constructed Co 3 N−Mo 0.2 /NF||Co 3 N−Mo 0.2 @FeOOH/NF electrolyzer exhibits a small voltage of 1.48 V to achieve 50 mA cm −2 at 80 °C, which is superior to most of the reported electrocatalysts. Rational design of efficient electrocatalysts is highly imperative but still a challenge for overall water splitting. Herein, we construct self-supported Co 3 N nanowire arrays with different Mo doping contents by hydrothermal and nitridation processes that serve as robust electrocatalysts for overall water splitting. The optimal Co 3 N−Mo 0.2 /Ni foam (NF) electrode delivers a low overpotential of 97 mV at a current density of 50 mA cm −2 as well as a highly stable hydrogen evolution reaction (HER). Density functional theory (DFT) calculations prove that Mo doping can effectively modulate the electronic structure and surface adsorption energies of H 2 O and hydrogen intermediates on Co 3 N, leading to improved reaction kinetics with high catalytic activity. Further modification with FeOOH species on the surface of Co 3 N−Mo 0.2 /NF improves the oxygen evolution reaction (OER) performance benefiting from the synergistic effect of dual Co−Fe catalytic centers. As a result, the Co 3 N−Mo 0.2 @FeOOH/NF catalysts display outstanding OER catalytic performance with a low overpotential of 250 mV at 50 1 mA cm −2 . The constructed Co 3 N−Mo 0.2 /NF||Co 3 N−Mo 0.2 @FeOOH/NF water electrolyzer exhibits a small voltage of 1.48 V to achieve a high current density of 50 mA cm −2 at 80 °C, which is superior to most of the reported electrocatalysts. This work provides a new approach to developing robust electrode materials for electrocatalytic water splitting.
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高影响因子
Nanoscale
·
2022
·Vol. 14
·期 19
·7322-7331
·
IF 8.307
Si-Qi Zhu,Jin-Cheng Shu,Mao-Sheng Cao
The upcoming 5G era will powerfully promote the development of intelligent society in the future, but it will also bring serious electromagnetic pollution. Thus, the development of efficient, lightweight and multifunctional electromagnetic shielding materials and devices is an important research hotspot around the world. Herein, a novel needlelike Co3O4/C array architecture is constructed from MOF precursor via a simple pyrolysis process, and its microstructure is controllably tailored by changing the pyrolysis temperature. The unique 3D hierarchical structure and multiphase components enable the architecture to provide high-efficiency electromagnetic interference (EMI) shielding, along with good thermal insulation. More importantly, the architecture possesses fast ion transport channels, which can be used to construct supercapacitors with high specific capacitance and excellent cycle stability. Obviously, this work offers a new inspiration for the design and construction of multifunctional electromagnetic materials and devices.
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EcoMat
·
2022
·Vol. 4
·期 2
·e12164
·
IF 12.213
Chaoyu Lin,Gan Luo,Huiqin Zhou,Anlin Feng,Li Zeng,Qingyang Li
An amorphous Ni nanoparticles-loaded ZnO nanowire array is controllably constructed on stainless steel mesh through combined electrodeposition and hydrothermal reaction. Its nano-arrayed structure not only provides a platform to achieve stable and good dispersion of Ni nanoparticles, but also helps improve their ability to adsorb 4-nitrophenolate ions and to capture hydrogen radicals, thereby accelerating the hydrogen transfer from metal hydride complex to 4-nitrophenol. Benefiting from the abovementioned unique features, it outperforms most Ni-based catalysts. While a 30-s re-electrodeposition of Ni can provide it extra 150 min of high catalytic activity towards the reduction of waste 4-nitrophenol to valuable 4-aminophenol, further demonstrating its outstanding reusability. The highly general methodology reported here paves the way to economically and effectively synthesize various other metal nanoparticles-loaded ZnO nanowire arrays on different conductive substrates, which not only enrich the nanowire-arrayed catalysts, but also significantly promote their practical utilizations in a wide range of environment-related fields.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Wensen Liu,Hui Su,Jian Zhang,Lina Wang,Yahui Liu,Jie Liang,Zhaowu Zhu
The hydrometallurgical process for the recovery of nickel and cobalt requires a complex and expensive impurity removal process. Solvent extraction is widely used in industry for the separation, purification, and concentration of metals. However, current commercial extractants encounter some difficulties when cobalt and nickel are extracted from solutions containing a large amount of impurities such as manganese and calcium. There is an urgent need to develop new reagents for the selective extraction of Ni and Co. In this study, N-(2-ethylhexyl)-pyridine-4-carboxamide (NEHPCA) was synthesized, and the metal extraction capacity of its synergistic solvent extraction (SSX) system with dinonylnaphthalene sulfonic acid (DNNSA) and tributyl phosphate (TBP) modifier was examined. The experimental results show that the selectivity of the new SSX system has the order Cu > Ni > Co > Zn > Mn > Ca > Al ≈ Cr (III) ≈ Mg ≈ Fe (III), with excellent selectivity for nickel and cobalt. Using an organic phase composed of 0.7 M NEHPCA, 0.35 M DNNSA, and 0.2 M TBP under 1:1O/A operation, after three-stage theoretical extraction, more than 99% of nickel and cobalt can be recovered from a synthetic leaching solution of nickel laterite ore. Mechanistic studies showed that NEHPCA and water molecules participate in the internal coordination of metals, and DNNSA provided coordination anions to achieve charge balance, forming the Ni complex in this SSX system which existed most likely in the form of [Ni(NEHPCA) 2 (H 2 O) 4 ](DNNS) 2 in the organic phase.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Yang Yu,Xiaoping Cai,Xinyang Jiao,Chengyi Xu,Jinan Niu,Peizhong Feng
Ni-Al-Cr intermetallic compounds are candidate at extreme environment due to their excellent oxidation resistance at high temperature, and the oxidation resistance of Ni-Al-Cr alloy system has been studied extensively. However, the research on oxidation resistance mechanism of porous Ni-Al-Cr intermetallic compounds is still not deep. In our work, porous Ni-Al-Cr intermetallic compounds were synthesized by thermal explosion, and the oxidation resistance of porous Ni-Al-Cr system was mainly investigated. The results indicate that Cr promotes the formation of highly protective continuous Al 2 O 3 layer, increasing the oxidation resistance at 900 °C of porous Ni-Al-Cr. After oxidation at 900 °C for 120 h, the minimum mass gain of Ni-Al-Cr products is only 6.96%.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Ruonan Zhang,Yanchao Xu,Liguo Shen,Renjie Li,Hongjun Lin
Efficient separation of oil-in-water emulsion remains a decisive step for success of oily wastewater treatment . To achieve this goal, a novel strategy regarding combining membrane separation with in situ electrocoagulation based on sacrificial anodes and cathodic hydrogen evolution via conductive metalized fabric membrane was proposed. As a key component of this novel coupling system, nickel functionalized fabric membrane with high hydrophilicity and electrical conductivity (electrical resistance of ∼2 Ω cm −1 ) was successfully prepared via a low-cost and facile route, including steps of PVA (polyvinyl alcohol)/Ni coating and autocatalytic electroless Ni plating. The optimized conductive membranes exhibited high permeate flux (19.3 × 10 5 L m −2 h −1 ·bar −1 ), separation efficiencies (99.5%), and separation stability to separate oil/water mixtures during the gravity-driven filtration process. To achieve the ideal performance to separate oil-in-water emulsion, a coupled electrocoagulation-membrane separation system was constructed with Ni@PVA membrane and Al mesh as the cathode and anode, respectively. It was shown that the coupled electrocoagulation-membrane separation system could achieve 99.4% rejection with high flux of 12.0 × 10 3 L m −2 h −1 ·bar −1 for oil/water emulsion separation, under the current density of 8 mA cm −2 and 20 min electrolysis time. This study revealed that the proposed electrocoagulation-membrane separation system based on Ni@PVA membrane is a promising technique in oil/water separation.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Xiaoyue Liu,Hongtao Xie,Jian Mao
The porous electrodes derived from Prussian blue analogs (PBAs) show high specific capacity and superior energy densities in supercapacitors due to their tunable chemical compositions, open three-dimensional network framework and large surface area. In this work, La-Fe PBA with different morphologies is prepared at mild conditions via controlling the composition of mixed solvent and the structural evolution of the La-Fe PBA is further explored. The solubility of K 3 [Fe(CN) 6 ] and the influence of ethanol on the crystal growth is used to control the synthesis of La-Fe PBA. Four different morphologies of La-Fe PBA, such as chamfered hexagonal bipyramid microcrystals, hexagonal flakes, erythrocyte-like microstructure and small flakes, are successfully synthesized by changing the ethanol/water ratio of mixed solvent. The porous LaFeO 3 with the same shape is obtained by calcining the La-Fe PBA at 500 °C, which is subsequently employed as electrodes for battery-type supercapacitor. The erythrocyte-like LaFeO 3 shows remarkable specific capacity (330 C g −1 ) at 1 A g −1 , energy density (23.8 Wh kg −1 ) and power density (400 W kg −1 ) at 1 A g −1 . This work could provide a porous material for high-performance supercapacitors as well as an exciting strategy to develop and design materials with specific morphology.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Wenjun He,Rui Zhang,Jingyu Zhang,Fangqing Wang,Ying Li,Jianling Zhao,Cong Chen,Hui Liu,Huolin L. Xin
Developing cost-effective non-precious electrocatalysts with excellent HER performance in alkaline media is of significance for industrial hydrogen production . Herein, we successfully endow Ni 3 S 2 with unprecedentedly enhanced alkaline HER activities by introducing nickel vacancies. The Ni 3 S 2 catalyst with nickel vacancies exhibits an ultralow overpotential of 35 mV at 10 mA cm −2 in 1 M KOH electrolyte, outperforming commercial Pt/C (56 mV) and most reported non-precious electrocatalysts. The electron paramagnetic resonance and X-ray absorption fine structure etc. validates the formation of Ni vacancies and the change of the geometric/electronic structure of Ni 3 S 2 . Additionally, the theoretical calculations reveal that the Ni sites with higher valence state neighbouring the Ni vacancies can promote the water dissociation, playing a vital role in accelerating HER kinetics in alkaline media. This work may provide a universal strategy to enhance the HER activity of transition-metal compound catalysts in alkaline media by means of cationic defect engineering.
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高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 4
·640
·
IF 5.719
Lin Bo,Fujin Li,Yangbo Hou,Min Zuo,Degang Zhao
Forming co-alloying solid solutions has long been considered as an effective strategy for improving thermoelectric performance. Herein, the dense Cu2−x(MnFeNi)xSe (x= 0–0.09) with intrinsically low thermal conductivity was prepared by a melting-ball milling-hot pressing process. The influences of nanostructure and compositional gradient on the microstructure and thermoelectric properties of Cu2Se were evaluated. It was found that the thermal conductivity decreased from 1.54 Wm−1K−1to 0.64 Wm−1K−1at 300 K via the phonon scattering mechanisms caused by atomic disorder and nano defects. The maximumzTvalue for the Cu1.91(MnFeNi)0.09Se sample was 1.08 at 750 K, which was about 27% higher than that of a pristine sample.Keywords:thermoelectric material;nanostructured;interfacial engineering;multi-scale scattering centers
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Lei Zuo,Junfeng Wang,Deqing Mei,Derick Adu-Mensah,Yaping Gao
The amounts of methyl stearate (C18:0) and trans-methyl oleate (trans-C18:1) increase during the catalytic transfer hydrogenation (CTH) process of biodiesel. Although it could improve the oxidation stability of biodiesel, its low temperature performance would be worsened. As for it, ultrasonic was introduced in the CTH to control the generation of C18:0 and trans-C18:1. In this study, the ultrasonic-assisted CTH was performed using Raney-Ni as catalyst, isopropanol as hydrogen donor and water as solvent. The effect of operating parameters such as reaction temperature, stirring rate, catalyst dosage, isopropanol amount and water amount on hydrogenation process was investigated. It was revealed that the optimum reaction conditions were determined as reaction temperature 80 °C, stirring rate 600 rpm, catalyst dosage 10 wt%, isopropanol amount 32 g and water amount 100 g in the aspect of the iodine value of bioidesel and the yield of C18:0 and trans-C18:1. The process of the ultrasonic-assisted CTH for biodiesel could be well described by pseudo-first order kinetic model. The conversion rate constants from C18:2 to C18:1 ( k 1 ) and from C18:1 to C18:0 ( k 2 ) were 0.02649 min −1 and 0.00438 min −1 , respectively. Ultrasonic field effectively repressed the selectivity of trans-C18:1 and further decreased the iodine value of biodiesel. On the basis of the same iodine value, the yield of C18:0 and hydrogenation time reduced with ultrasonic. Overall, ultrasonic is an effective intensification method for the CTH of biodiesel in the aspect of product selectivity and reaction rate.
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MATERIALS CHARACTERIZATION
·
2022
·
IF 4.537
Z. Sun,X.X. Zhu,H.Z. Chen,L.X. Zhang
To address the excessive formation of brittle compounds when brazing TiAl alloys, a TiZrHfCoNiCu high-entropy brazed filler was developed to realize the brazing of TiAl/Ti 2 AlNb couples. The TiAl/Ti 2 AlNb brazed joints can be divided into 4 zones, i.e., 2 diffusion zones at the TiAl/braze filler, Ti 2 AlNb/braze filler interfaces and 2 zones divided inside the brazed seam. α 2 + γ-TiAl were the main reaction products formed at the TiAl/braze filler interface and α 2 + Ti 0.5 Al 0.12 Nb 0.38 were the main reaction products at the Ti 2 AlNb/braze filler interface. Effects of brazing temperatures on the interfacial microstructure and mechanical properties of the TiAl/Ti 2 AlNb brazed joints were investigated. When brazing at 1100°C/15 min, the highest shear strength can reach 157 MPa (room temperature), and 123 MPa (650°C) respectively. The relationship between the microstructure and the corresponding mechanical response were discussed in detail. This research can offer new insights on developing desirable brazing filler when joining TiAl and TiAl based alloys.
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