CHEMICAL ENGINEERING & TECHNOLOGY
·
2017
·Vol. 41
·期 2
·353-366
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IF 2.051
Shumin Wang,Qingping Guo,Shujun Liang,Peng Li,Xin Li,Jujie Luo
For the evaluation of CH 4 /N 2 separation, mixed-matrix membranes (MMMs) were fabricated by adding [Ni 3 (HCOO) 6 ] as a filler into the poly(styrene- b -butadiene- b -styrene) (SBS) polymer. The structures and morphologies of [Ni 3 (HCOO) 6 ] and [Ni 3 (HCOO) 6 ]/SBS MMMs were characterized by different techniques, proving the crystalline structure of [Ni 3 (HCOO) 6 ] in SBS polymer matrices. The structural integrity of the MMMs and good compatibility between [Ni 3 (HCOO) 6 ] and SBS polymer were examined by scanning electron microscopy. Gas permeation measurements revealed that membranes containing various [Ni 3 (HCOO) 6 ] loadings exhibited different separation performances. The operational temperature exerted a significantly positive effect on the separation of CH 4 and N 2 .
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ACS Catalysis
·
2026
·
IF 13.6
Jiaqing Liu,Xiaoqing Liu,Jiacheng Zhang,Zheng Liang,Wei Lin,Xue Feng Lu
Achieving high current densities with nickel-based catalysts within the urea oxidation reaction (UOR) potential window is critical for the scalable implementation of urea electrolysis. However, their performance is limited by the high energy barriers of Ni2+ deprotonation and sluggish proton-coupled electron transfer (PCET) processes. Herein, ultrafine PtNi-Ni nanoparticles rooted on porous TiO2 (PtNi-Ni/TiO2) nanotubes are constructed by a facile surface segregation and galvanic replacement reaction. The obtained PtNi-Ni/TiO2 electrocatalysts deliver the highest UOR current density of 284.4 mA cm–2 at a low potential of 1.50 V, ranking among the top UOR electrocatalysts reported. Kinetic analysis and theoretical calculations reveal that alloying significantly reduces the free energy for the Ni2+ electrooxidation, while heterojunction engineering promotes the PCET process and weakens the strong adsorption of urea, thereby improving the UOR current density. Moreover, PtNi-Ni/TiO2 delivered hydrogen evolution activity, enabling a urea electrolyzer employing PtNi-Ni/TiO2 as both anode and cathode to achieve 50 mA cm–2 at a low cell voltage of 1.55 V, which reduces the energy consumption by 17.2% compared with water splitting systems. This study provides a fundamental paradigm and insights for designing advanced nickel-based electrocatalysts for urea-splitting systems.
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RARE METALS
·
2025
·
IF 11
Han Ya,Yu Ying-Jian
Tin–air batteries (TABs) exhibit high safety and low cost, and are expected to be used in electric vehicles and portable electronic devices. However, challenges such as the irregular deposition of tin (Sn) particles on Sn anodes, surface passivation, and significant hydrogen evolution have hindered the development of high-performance TABs. To address these challenges, this study introduces quasi-solid TABs (QSTABs) with satisfactory high-temperature resistance. A conductive metal–organic framework (c-MOF), particularly Ni 3 (HITP) 2 , was synthesized and deposited onto the Sn anode surface. The porous structure of c-MOF increased the specific surface area of the Sn anode, improved electronic conductivity and facilitated the absorption and release of ions during charge and discharge cycling. Theoretical calculations revealed that Ni 3 (HITP) 2 provided more electron donor sites to coordinate with Sn 2+ and inhibited hydrogen release. Additionally, carboxymethyl cellulose (CMC) was incorporated into the organic gel polymer electrolytes (OGPEs) to significantly enhance their water retention, ensuring stable operation of QSTABs between 25 and 50 °C. Notably, QSTABs assembled with CMC-OGPE/Sn@Ni 3 (HITP) 2 exhibited a fine cycle life of over 200 cycles at 50 °C. The electronic c-MOF material effectively inhibited metal shedding and side reactions on the Sn anode. These findings provide valuable guidance for developing QSTABs with high-temperature resistance. Graphical abstract
研究领域:
储能
·
材料科学
·
电化学
·
电池技术
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VACUUM
·
2022
·
IF 4.11
Chang Xu,Jian Zhang,Huanjun Lu,Xiao Li,Jingchun Lv,Shaohui Zhang
In this work, one-dimensional (1D) conductive MOFs Ni 3 (HHTP) 2 with nanorod-like morphology on the surface of a woven fabric was synthesized by an in-situ growth method. Based on a three-electrode system, the effects of substrate concentration, scan rate and current density on electrode properties were investigated, respectively. The results showed that Ni 3 (HHTP) 2 @ woven fabric-3 (NHWF-3) demonstrated the largest area capacitance at 5 mV s −1 and reached up to 360 μF cm −2 at 20 μA cm −2 . Most importantly, the material still maintained 58.3% (210 μF cm −2 ) of the initially areal specific capacitance when the current density was increased 5 times to 100 μA cm −2 . According to the electrochemical impedance spectroscopy (EIS) curve, NHWF-3 has the smallest semicircle radius in the high-frequency region, indicating that it has the lowest internal transfer resistance and the best conductivity. Thus, this study provides a good example for the simple preparation and practical applications of conductive MOFs composites.
研究领域:
材料科学
·
电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Zhaohui Yang,Baolong Zhang,Chuanyu Yan,Zhimin Xue,Tiancheng Mu
Electrochemical oxidation is a promising method to convert 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) with high selectivity at room temperature. Developing catalysts with high current densities is crucial for the industrial application of HMF electrooxidation reaction (HMFOR). Herein, we demonstrate that the current densities exhibited by the LSV curves are falsely high and propose to evaluate catalyst activity using anodic peak current density rather than overpotential for the comparison of actual efficiency. Besides, the reduction of Ni 3+ to Ni 2+ accompanied by proton coupled electron transfer (PCET) process of HMF dehydrogenation is confirmed as the rate-determining step affecting the conversion efficiency of HMF rather than Ni 2+ electrooxidated to Ni 3+ . Theoretical calculations reveal differences in the hydrogen transfer energy barriers of PCET process. Furthermore, Ni(OH) 2 /NF with appropriate Cr doping shows superb activity with actual current densities of over 230 mA cm −2 at HMF concentrations of 10 mM and over 360 mA cm −2 at 20 mM (the ever highest current densities for HMFOR), and obtain a yield of more than 98% of FDCA.
研究领域:
电化学
·
催化材料科学
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Functional Materials Letters
·
2018
·
IF 1.084
Jujie Luo,Xing Yang,Shumin Wang,Yuhong Bi,Amit Nautiyal,Xinyu Zhang
The metal organic framework (MOF) [Ni 3 (HCOO) 6 ] was synthesized via the simple and fast microwave method, and the effect of irradiation power on crystallinity of synthesized Ni-based MOF was studied. The samples were characterized by using Fourier Transform Infrared Spectroscopy (FTIR), X-ray diffraction (XRD), and scanning electron microscopy (SEM). The synthesized Ni-based MOF was electrochemically characterized by using galvanostatic charge–discharge (GCD), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS) techniques. The synthesized MOF showed the highest specific capacitance of 1196.2 F/g at 1 A/g with excellent cyclability (86.04% capacitance retention after 2,000 cycles), thereby demonstrating its potential application in supercapacitors.
研究领域:
材料科学
·
电化学
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Liyan Wu,Jianmei Cen,Asad Ali,Jiecai Li,Pei Kang Shen
Conducting polymers are commonly used as precursors for preparing carbon-based catalysts and have been used in electrocatalytic water splitting. However, so far, most of the catalytic materials synthesized with the assistance of high polymer conducting polymers are non-self-supporting and have only a single-function catalytic effect. Therefore, it is an inevitable trend to synthesize a bifunctional self-supported, highly efficient and long-stable water splitting catalyst. Herein, a self-supporting polypyrrole precursor PPy-PW 12 was prepared by electrodeposition with phosphotungstic acid as a dopant. In addition, the PPy-PW 12 precursor was then calcined. The as-prepared W/Ni 3 (PO 4 ) 2 @NC/NF electrocatalyst exhibits admirable HER and OER performances with overpotentials of 48 mV for HER and 236 mV for OER to reach a current density of 10 mA cm −2 in 1.0 M KOH solution. Additionally, when W/Ni 3 (PO 4 ) 2 @NC/NF is used in overall water splitting as a bifunctional catalyst, it needs only 1.53 V to deliver a current density of 10 mA cm −2 , which is superior to typically integrated Pt/C and RuO 2 counterparts. Our work offers a facile strategy to apply W/Ni 3 (PO 4 ) 2 @NC/NF as practical bifunctional electrocatalysts for large-scale water splitting.
研究领域:
电化学
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材料科学
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催化
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能源材料
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Xupo Liu,Ran Wang,Mengyun Wei,Xihui Wang,Jiayao Qiu,Jingru Zhang,Shilong Li,Ye Chen
Electrochemical oxidation of biomass-based 5-hydroxymethylfurfural (HMF) is an effective approach for achieving the high-value products of 2,5-furandicarboxylic acid (FDCA). However, the restricted formation of high-valence metal active species for electrocatalysts results in a sluggish kinetic process of HMF oxidation reaction (HMFOR). Herein, we fabricated the Ni 3+ -rich cross-linked α-Ni(OH) 2 nanosheets for accelerating the HMFOR through an anion-mediated strategy. It is identified that the Cl − ions with strong penetrability replace a portion of lattice oxygen atoms in α-Ni(OH) 2 to form Ni-Cl bonds, contributing to breaking the inherent lattice order and generating a special Ni 3+ -rich structure. Owing to the promoted adsorption and accelerated oxidation of hydroxyl and aldehyde groups by the affluent Ni 3+ active species, the large oxidation current density of 116.5 mA cm −2 and HMFOR kinetic constant of 0.067 min −1 has been achieved at 1.45 V (vs. RHE). By analyzing the oxidation products, the FDCA yield and Faradic efficiency are both higher than 99.25 % and 99.36 % for five successive determinations. Therefore, this work provides an insightful anion-mediated strategy for designing high-performance electrocatalysts for biomass conversion application.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xin-yue Lan,Zhi Huang,Yan-ying Liu,Jun-ming Hong,Qian Zhang
Electron transfer capability as crucial properties of anode is directly related to electrocatalytic performance. However, the contributions of electron transfer were always under estimated due to the ambiguous mechanism of electrocatalysis. In this paper, a new electron transfer bridge was constructed in Ni 3 (HTTP) 2 /GO to provide a new insight into electrocatalytic performance enhancement. The contributions of active sites candidates, including metal sites, ligands (metal bridging atoms), and electron transfer bridges were innovatively separated. As replacement experimental results (of metal sites and metal bridging atoms), both metal sites and metal bridging atoms contributed slightly as the active center directly for the electrocatalytic degradation of tetracycline hydrochloride (TCH). The great improvement was attributed to the generation of “GO-C-O-S-C-Ni 3 (HTTP) 2 ” bridges, in which S atoms from ligands were critical anchoring sites for the connection of two 2D layers (Ni 3 (HTTP) 2 and GO layer). The experimental and density functional theory results showed Ni 3 (HTTP) 2 could donate electrons to GO layers, leading the electrostatic imbalance of charge density to facilitate electron withdrawal from pollutions (not only TCH, but also dyes and complex microbial flora). The results of this paper provide a new strategy for improving electrocatalytic efficiency by adjusting electron transfer for novel practical applications of Ni 3 (HTTP) 2 /GO composites.
研究领域:
电化学
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催化
·
材料科学
·
环境科学
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JOURNAL OF MOLECULAR STRUCTURE
·
2026
·
IF 4.9
Ping Zhang,Qin-Wen Shi,Wen-Yuan Wu,Jun-Feng Bai
An anionic 3D MOF featuring 9-connected Ni 3 ( μ 3 -OH) secondary building units (SBUs), (Me 2 NH 2 ) 2 [Ni 6 (OH) 2 (Bpdc) 3 (4-Ptz) 6 ]·11H 2 O (NJTU-Bai90; NJTU-Bai denotes Nanjing Tech University Bai’s group), was hydrothermally synthesized using the bifunctional ligands bicyclo[1.1.1]pentane-1,3-dicarboxylic acid (H 2 Bpdc) and 4-(2H-tetrazol-5-yl)pyridine (4-HPtz). This MOF crystallizes in I-43 m space group and possesses intersecting 3D channels packed by trigonal-pyramidal and tetrahedral cages. Tailored for reversible C 2 H 6 adsorption and one-step purification of polymer-grade C 2 H 4 , NJTU-Bai90 not only has a high BET surface area of 1465.7 m 2 g −1 but also exhibits excellent stability in aqueous solutions at room temperature for at least one month. NJTU-Bai90 exhibits superior C 2 H 6 uptake (97.6 cm 3 g −1 at 298 K and 82.5 cm 3 g −1 at 308 K, both measured at 1 bar) in comparison with C 2 H 4 (85.5 cm 3 g −1 at 298 K and 68.4 cm 3 g −1 at 308 K, both measured at 1 bar). Remarkable IAST selectivity values (1.51 and 1.56, respectively) are maintained even at elevated temperatures. Furthermore, dynamic breakthrough experiments demonstrate that a C 2 H 6 /C 2 H 4 mixture (1/15, v/v) can be efficiently separated in one step and that polymer-grade C 2 H 4 yielding with a productivity of 19.1 mL g −1 at 298 K and 1 bar. The distinct retention times of C 2 H 6 and C 2 H 4 on NJTU-Bai90-packed separation columns further highlight the material’s great potential for industrial gas separation applications.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Jin Zhao,Tianxiang Jiang,Junrui Cao,Xuemin Feng,Xunliang Wang,Baolong Xie,Yuhui Ma,Huafeng Ren,Yu Cheng,Keyuan Zhang,Yutong Han,Xianghai Guo,Yizhong Zhang
Mild hydrothermal strategy well preserves abundant O/N functional groups of Chitosan-derived amorphous carbon. • Chitosan-derived amorphous carbon efficiently stabilizes intrinsic Ni 3+ active sites. • Pre‑stabilized intrinsic Ni 3+ promotes the reconstruction of γ‑NiOOH. • Interfacial electronic modulation lowers UOR overpotential and delivers remarkable UOR activity. Replacing the sluggish oxygen evolution reaction (OER) with the urea oxidation reaction (UOR) offers a promising route for energy-efficient hydrogen production and the electrochemical treatment of urea-containing wastewater. However, the practical application of UOR is still hindered by insufficient anode durability and sluggish UOR kinetics. Herein, biomass chitosan was employed as the carbon precursor to fabricate amorphous carbon-modified coral-like NiFe layered double hydroxide (NiFe-LDH), which was in-situ anchored on nickel foam via a facile one-step hydrothermal strategy. The optimized catalyst achieved remarkable UOR electrocatalysis, requiring only 0.94 V and 0.96 V overpotential to reach 50 mA·cm −2 and 100 mA·cm −2 , respectively, accompanied by a small Tafel slope of 22 mV·dec −1 and outstanding long-term stability exceeding 1000 h at 100 mA·cm −2 . Operando spectroscopic characterizations and density functional theory (DFT) calculations indicated that electron-withdrawing functional groups on chitosan-derived amorphous carbon induced interfacial electron transfer, which stabilized electron-deficient Ni 3+ sites. This pre-stabilized Ni 3+ facilitated the in-situ generation of active γ-NiOOH at low potential, while γ-NiOOH served as the catalytic phase to drive the UOR; the complementary synergy between the two significantly enhanced the overall catalytic performance. This study affords a versatile interfacial modulation protocol for designing high-performance crystalline/amorphous hybrid electrocatalysts, which may offer a promising route for sustainable energy conversion and the electrochemical treatment of urea-containing wastewater. Download: Download high-res image (213KB) Download: Download full-size image Electron-withdrawing O/N groups of chitosan-derived amorphous carbon tunes Ni and Fe 3d- t 2 g orbitals of NiFe-LDH via interfacial charge transfer, stabilizing intrinsic Ni 3+ and reducing UOR overpotential.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Zongyang Peng,Zhuang Zuo,Qi Qi,Shaocong Hou,Yongping Fu,Dechun Zou
Nickel oxide (NiOx) is widely used as a promising hole transport material for perovskite solar cells (PSCs). A high concentration of Ni3+ in the NiOx film is generally beneficial for charge transport of the PSCs; however, chemical redox reactions between surface Ni3+ and perovskite materials result in decomposition of perovskite materials, which causes carrier recombination and impedes charge transport at the perovskite–NiOx interface. Herein, we employ magnetron sputtering to fabricate NiOx thin films with adjustable Ni3+ concentrations to optimize the hole-transporting properties. A thin layer of phenylethylamine iodide (PEAI) is further introduced to reduce the detrimental Ni3+ at the surface of NiOx, which eliminates the formation of undesirable defects and chemical species when in contact with the perovskite layer, leading to a dramatic increase in the power conversion efficiency (PCE) from 16.37 to 20.01%, which is one of the best performance using sputtered charge transport layers. The unencapsulated devices retain 88% of their initial PCE after storage in a nitrogen atmosphere for 1000 h under light. We further perform solar cell capacitance simulator (SCAPS) simulation to understand the effects of bulk and interfacial charge transport on the performance of PSCs, which agree with our experimental results. This work not only highlights the double-edged sword effect of the Ni3+ content on the performance and stability of PSCs but also demonstrates a simple yet effective strategy to avoid the undesirable reaction between Ni3+ and perovskite materials in the fabrication of PSCs with sputter-deposited NiOx.
研究领域:
材料科学
·
能源科学
·
光电化学
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高影响因子
危险品化学品经营许可证（带存储）