DALTON TRANSACTIONS
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2022
·Vol. 51
·期 26
·10061-10068
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IF 4.569
Congli Wang,Hongfang Jiu,Lixin Zhang,Wei Song,Yufang Zhang,Hao Wei,Qianwen Xu,Yaqi Qin,Sicong Che,Zhixin Guo
It is of utmost importance to explore bifunctional electrocatalysts for water splitting. Herein, unique ZnCo2O4–CoOOH heterostructured ultrathin nanosheets on Ni foam are reported that combines a two-step hydrothermal method. This catalyst exhibits excellent catalytic performances to achieve a current density of 10 mA cm−2 with an ultralow overpotential of 115 mV for HER, attaining an overpotential of 238 mV at 20 mA cm−2 for OER. Remarkably, ZnCo2O4–CoOOH/Ni shows a voltage of 1.494 V to drive a current density of 10 mA cm−2. Such performances are due to the inter-penetrative pores present in the ultrathin nanosheets that provide large surface areas and expose massive active sites to enhance activities. In addition, the unique nanosheet structure and the 3D Ni foam substrate possess large specific surface areas, which can facilitate mass diffusion. This excellent performance is ascribed to the ZnCo2O4–CoOOH heterostructure that manipulates strong synergy to improve the electrochemical activity. This study offers new insight on an innovative approach for the exploitation of effective bifunctional electrocatalysts with a heterostructure.
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CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Zhufeng Hu,Yinxiang Xu,Wenchao Xiang,Xiaodong Guo,Yuchen Tong,Junbo Xu,Chao Yang
The oxygen evolution reaction (OER) is the key to prepare electrocatalysts for water splitting. Heteroatom doping is an effective way to improve the catalytic performance of OER by modulating the local electronic environment and stimulating the synergy. However, the complicated manufacturing methods have hindered their practical application. Herein, we demonstrate a method based on FeOOH/CC precursor to realize the preparation of Ni-P-S@FeOOH/CC catalyst through fast electrodeposition method. The overpotential of Ni-P-S@FeOOH/CC catalyst is 210 mV (10 mA cm −2 ), and still has an initial voltage of 97.35 % for 48 h. The surface area analysis shows a higher electrochemically active surface area for the amorphous structure prepared by electrodeposition method. XPS and DFT results show that the co-doping of P and S can stimulate the synergistic effect and the minimum energy of adsorption/desorption in OER process is only 0.83 eV. The strategy shows good prospects for preparing efficient OER pre-catalysts.
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INORGANIC CHEMISTRY
·
2022
·
IF 5.436
Si-Jia Guan,Peng Zhang,Shen-Jing Ji,Yu Cao,Nian-Tzu Suen
It is well known that the “iron” impurity will influence the oxygen evolution reaction (OER) in an alkaline electrolyte, especially for the Ni-based electrocatalyst. Many research studies have investigated the function of Fe in the OER active phase, such as M(OH)2/MOOH (M = Ni and/or Fe), while, surprisingly, very few studies have examined the function of Fe in the “precatalyst” system. Accordingly, in this work, the Ni3–xFexP (x = 0, 0.5, 1) series as an Ni-based precatalyst was employed to inspect the function of internal and external Fe in the Ni-based precatalyst system. It was realized that the sample with internal Fe (i.e., Ni2.5Fe0.5P and Ni2FeP) exhibits efficient OER activity compared to that of the Fe-free one (i.e., Ni3P) owing to the large amount of active M(OH)2/MOOH formed on the surface. This indicates that the internal Fe in the present system may have the ability to facilitate the phase transformation; it was later rationalized from electronic structural calculations that the d band center of the internal Fe (middle transition metal) and Ni (late transition metal) holds the key for this observation. Adding excessive ferrous chloride tetrahydrate (FeCl2·4H2O) as the external Fe in the electrolyte will greatly improve the OER performances for Ni3P; nevertheless, that the OER activity of Ni2FeP is still much superior than that of Ni3P corroborates the fact that the Fe impurity is not the only reason for the elevated OER activity of Ni2FeP and that internal Fe is also critical to the phase transformation as well as OER performance.
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CHEMOSPHERE
·
2022
·
IF 8.943
Tao Zhang,Pan Wu,Gary Owens,Zuliang Chen
Since ofloxacin (OFX) is one of many common antibiotics, which effluxes into aquatic environment in relatively high concentration, it has become of significant environmental concern due to the potential for increased antibiotic resistance. In this study, an innovative functional Fe/Ni@ZIF-8 composite was successfully used for the Fenton-like oxidation of OFX, with a OFX removal efficiency >98% under optimal conditions. FTIR analysis confirmed that OFX removal occurred via adsorption to Fe/Ni@ZIF-8 by a combination of π-π bond intercalation and electrostatic interaction, while XPS revealed that the Fe/Ni NPs in Fe/Ni@ZIF-8 were also involved in oxidation. Furthermore, LC-MS analysis identified the presence of several OFX degradation products post exposure, which indicted that Fe/Ni NPs in Fe/Ni@ZIF-8 reacted with H 2 O 2 to form •OH, leading to Fenton-like oxidation of OFX. Thus overall, OFX removal by Fe/Ni@ZIF-8 involved both adsorption to ZIF-8 and Fenton-like oxidation by Fe/Ni NPs. A synergistic mechanism for OFX removal by Fe/Ni@ZIF-8 was thus proposed. The removal efficiency of the synthesized catalysts remained high (above 65%) even after a 5th reuse cycle, which reflected the high stability of Fe/Ni@ZIF-8. Overall, this study demonstrated that Fe/Ni@ZIF-8 had significant potential for the removal of OFX from wastewaters with a removal efficiency >90%.
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Molecular Catalysis
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2022
·
IF 5.089
Xiaoyuechuan Ma,Shishuai Shi,Qixiang Xu,Li Xu,Guoji Liu
As an important intermediate of organic chemical industry, 2-methylnaphthalene (2-MN) has the application value in the field of medicine and material research. Up to date, the existing researches are aimed at 2-methylnaphthalene saturated hydrogenation and hydrocracking for high value products such as cycloalkanes and BTXs. A series of Ni-based (20 wt.%) catalysts were prepared with different reduction temperatures for the hydrogenation of 2-methylnaphthalene to 6-methyl-1,2,3,4-tetrahydronaphthalene (6-MT) in this study. The results showed that by using NiO/Al 2 O 3 -370R, 90.8% conversion of 2-MN and 59.7% yield of desired product (6-MT) can be achieved with optimum reaction conditions of 4 MPa & 340°C, 8 h. Multiple studies including catalyst characterizations, reaction kinetics and density functional theory (DFT) calculation indicates that symbiotic effect of heterostructured Ni-NiO over γ-Al 2 O 3 mainly corresponding to the desired catalytic performance. This study gains fundamental understanding in the effects of valence of Ni-based catalysts in catalytic hydrogenation.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Qiulin Li,Ke Zhang,Xiang Li,Jiaqi He,Yongbing Lou,Jinxi Chen
The creation of considerably effective electrocatalysts to reduce overpotentials is essential for speeding up the sluggish oxygen evolution reaction (OER) processes, which is imperatively required for the practical exploitation of electrochemical water-splitting. Herein, we prepared a unique composite structure, uniformly spherical Ni-MOF decorated with NiMoO 4 nanorods on Ni foam (NF), and assessed its performance toward oxygen evolution reaction. The synergistic effect between NiMoO 4 and Ni-MOF remarkably promoted the OER intrinsic activity. Moreover, introducing NiMoO 4 endowed the composite structure with enhanced electrical conductivity and exposed more active sites. The NiMoO 4 /Ni-MOF/NF electrode exhibited exceptional electrocatalytic activity in 1.0 M KOH aqueous solution, with a low overpotential of 218 mV to drive the current density of 10 mA cm −2 and a low Tafel slope (67.75 mV dec −1 ), surpassing the benchmark RuO 2 . The presented strategy opens a promising candidate for preparing novel non-precious metal OER electrocatalysts derived from MOF materials for sustainable energy applications.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
·
IF 8.91
Xiaoying Jin,Heng Li,Xiuduan Zhu,Na Li,Gary Owens,Zuliang Chen
The integration of metal–organic frameworks with other functional materials has recently emerged as a promising approach for creating innovative materials for environmental remediation. Here, a nano-sized iron/nickel (Fe/Ni) functionalized zeolitic imidazolate framework-8 (ZIF-8-Fe/Ni) was fabricated for oxytetracycline (OTC) removal from wastewater. Cyclic voltammetry and amperometric I-t measurements indicated that OTC was degraded by ZIF-8-Fe/Ni. X-ray diffraction spectroscopy (XRD), transmission electron microscopy mapping (TEM-mapping) and X-ray photoelectron spectroscopy (XPS) indicated that Fe/Ni was evenly dispersed throughout ZIF-8 and partially oxidized after reaction with OTC. OTC adsorption isotherms and kinetics best fitted the Langmuir isotherm ( R 2 > 0.982) and pseudo-second-order model ( R 2 > 0.997), respectively. Reduction kinetics data followed the pseudo-first-order model ( R 2 > 0.905), where the apparent activation energy ( E a) was 22.9 kJ mol −1 , demonstrating that OTC degradation was mainly via a chemical process. The practical removal efficiency of OTC from real wastewater by ZIF-8-Fe/Ni was 92.6%, where even after application of ZIF-8-Fe/Ni for 5 consecutive removal cycles, a high OTC removal of 74.9% was maintained. Thus ZIF-8-Fe/Ni exhibited both high removal efficiency and good recyclability .
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Nanomaterials
·
2022
·Vol. 12
·期 15
·2550
·
IF 5.719
Yuqian Yu,Li Kang,Lixian Sun,Fen Xu,Hongge Pan,Zhen Sang,Chenchen Zhang,Xinlei Jia,Qingli Sui,Yiting Bu,Dan Cai,Yongpeng Xia,Kexiang Zhang,Bin Li
Sodium borohydride (NaBH4), with a high theoretical hydrogen content (10.8 wt%) and safe characteristics, has been widely employed to produce hydrogen based on hydrolysis reactions. In this work, a porous titanium oxide cage (PTOC) has been synthesized by a one-step hydrothermal method using NH2-MIL-125 as the template and L-alanine as the coordination agent. Due to the evenly distributed PtNi alloy particles with more catalytically active sites, and the synergistic effect between the PTOC and PtNi alloy particles, the PtNi/PTOC catalyst presents a high hydrogen generation rate (10,164.3 mL∙min−1∙g−1) and low activation energy (28.7 kJ∙mol−1). Furthermore, the robust porous structure of PTOC effectively suppresses the agglomeration issue; thus, the PtNi/PTOC catalyst retains 87.8% of the initial catalytic activity after eight cycles. These results indicate that the PtNi/PTOC catalyst has broad applications for the hydrolysis of borohydride.Keywords:hydrogen generation;porous titanium oxide cage;PtNi nanoparticles;sodium borohydride hydrolysis
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JOURNAL OF CHEMICAL SCIENCES
·
2022
·Vol. 134
·期 3
·1-9
·
IF 2.15
Bao Wanting,You Junhua,Zhao Yao,Wang Lu,Yao Ruyue
Electrochemical water splitting has excellent application prospects in clean energy technology. However, due to the large overpotential required for the OER reaction during the water-splitting reaction, the modification of electrocatalysts is a vital strategy to address the slow kinetics of the OER reaction. In this paper, a simple and rapid two-step hydrothermal sulfidation method was used to prepare S-modified Ni(OH) 2 nanosheets electrocatalysts at 120 °C. At the same time, the well-designed nanostructured catalyst on the nickel foam substrate exposes a large number of active sites, and the simultaneously generated oxygen vacancies are beneficial to the penetration of the electrolyte and release of O 2 , thus significantly improving the OER performance. In 1.0 M KOH electrolyte, Ni 9 S 8 /Ni(OH) 2 /NF exhibits excellent catalytic activity for OER. The catalyst requires only 430 mV overpotential at a current density of 100 mA cm -2 . In addition, Ni 9 S 8 /Ni(OH) 2 /NF also has excellent long-term stability. Graphical abstract This work reports the formation of Ni 9 S 8 /Ni(OH) 2 /NF heterojunctions by sulfiding Ni(OH) 2 on porous nickel foam. Surprisingly, these Ni 9 S 8 /Ni(OH) 2 /NF heterojunctions exhibit excellent oxygen evolution reaction performance and long-term stability. This is superior to most reported electrocatalysts for oxygen evolution reactions.
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Inorganic Chemistry Frontiers
·
2022
·Vol. 9
·期 22
·5982-5993
·
IF 7.779
Yifan Pan,Dongyan Gao,Yupeng Dang,Pengcheng Xu,Dandan Han,Changling Liu,Yen Wei,Yanru Yang
Metal–organic frameworks (MOFs) with bimetallic centers are considered as promising electrode materials for supercapacitors due to the large specific surface area and potential redox sites. In this work, the internal structure evolution, electron transfer in the metal center, and the mechanism of action of the Mn dopant to enhance conductivity in electrochemical processes are discussed. Density functional theory (DFT) calculations show that the introduction of Mn ions greatly reduces the band gap of the Ni-MOF and increases the carrier concentration, confirming the electron transfer process of electrons from Ni2+ to Mn2+ through the bridging oxygen. Therefore, the optimal NiMn-MOF produces an impressive specific areal capacity of 1.89 mA h cm−2 at 1 mA cm−2. Meanwhile, a hybrid supercapacitor (HSC) based on the NiMn-MOF electrode and activated carbon (AC) can output a high specific energy of 67.5 W h kg−1 at a specific power of 84.5 W kg−1 with excellent cycling stability (capacity retention of 94% after 10 000 cycles). Taking advantage of the high-energy storage properties of the NiMn-MOF//AC supercapacitor device, a solar power generation system is further integrated for self-powered portable electronic applications. This work broadens the applicability of activity prediction for bimetallic MOF electrode materials with high electrochemical performance.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jing Feng,Gang Lang,Tingting Li,Jing Zhang,Jun Zhao,Wei Li,Weiqing Yang,Zhenju Jiang
Coordination-driven self-assembly has emerged as a smart strategy to prepare advanced materials for various applications. Here we coat Ni(II)-tannic acid complexes on the lab-made C-Cr 2 O 3 nanoparticles by this strategy, and demonstrate that this novel coating dramatically accelerate the charge transfer and thus enhance the amperometric responses for electrochemical detection of glucose and hydrazine. The charge-transfer rate ( k s ) of the obtained C-Cr 2 O 3 @Ni-MPN is much higher than that of C-Cr 2 O 3 substrate, evaluated as 1.00 and 0.82 s −1 respectively. The physicochemical and electrochemical characterizations demonstrate that the enhanced k s of C-Cr 2 O 3 @Ni-MPN is attributed to the electronegativity and the network structure of its surface. Correspondingly, C-Cr 2 O 3 @Ni-MPN exhibits superior sensitivity (5043.3 μA mM −1 cm −2 ) and ultra-low detection limit (0.02 μM) for the glucose detection, as well as high sensitivity (918.5 μA mM −1 cm −2 ) and ultra-low detection limit (0.04 μM) for the hydrazine detection. Furthermore, C-Cr 2 O 3 @Ni-MPN exhibits the excellent selectivity, stability and reproducibility, and the powerful reliability for analyzing the plasma samples. This study constructs an appropriate hierarchical structure towards catalyzing the electrochemical oxidation of targets, which achieves the amplification of the respond current and thus an ultra-sensitive electrochemical detection for the targets.
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Beilei Cui,Hua Wang,Jinyu Han,Qingfeng Ge,Xinli Zhu
The relatively cheap and abundant Ni as a catalyst for hydrodeoxygenation (HDO) of biomass lignin-derived phenolics at 350 °C and atmospheric pressure suffers from unfavorable C-C hydrogenolysis toward CH 4 with a lower direct deoxygenation (DDO) activity. Herein, we demonstrate that the activity and selectively of Ni for HDO of m-cresol can be modified through the differences of strong metal-support interaction (SMSI) on anatase and rutile TiO 2 . Characterizations showed that the presence of SMSI depended strongly on the crystal phase of TiO 2 . The SMSI dominates on Ni/a-TiO 2 after reduction at 350 °C, resulting in Ni particles partially covered by a TiO x overlayer, and this overlayer became sufficiently thick at 650 °C, causing a significant reduction of CO chemisorption. Although the catalyst became selective for DDO to toluene, the overall HDO activity was significantly reduced because of excessive SMSI. In contrast, the Ni/r-TiO 2 catalyst reduced at 350 °C exhibited little SMSI and was active for C-C hydrogenolysis like a bare Ni catalyst. Increasing reduction temperature to 650 °C, the Ni/r-TiO 2 catalyst showed moderate SMSI and became selective to toluene through DDO while completely inhibited CH 4 formation. The toluene and total aromatics yields were 84.8 and 92.2%, respectively, at full conversion. More importantly, the turnover frequency for DDO (2.43 min −1 ) on the Ni/r-TiO 2 catalyst reduced at 650 °C was ∼40 and ∼14 times higher than that of Ni on rutile and anatase, respectively, reduced at 350 °C. This study provides an example of “Goldilocks principle” in catalysis, i.e., the best performing catalyst offers a balanced SMSI!
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