ADVANCED MATERIALS
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2022
·Vol. 35
·期 5
·2205262
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IF 32.086
Runyao Zhao,Yiding Wang,Guipeng Ji,Jiajun Zhong,Fengtao Zhang,Meifang Chen,Shengrui Tong,Peng Wang,Zhonghua Wu,Buxing Han,Zhimin Liu
Electrocatalytic CO 2 reduction reaction (CO 2 RR) offers a promising strategy to lower CO 2 emission while producing value-added chemicals. A great challenge facing CO 2 RR is how to improve energy efficiency by reducing overpotentials. Herein, partially nitrided Ni nanoclusters (NiN x ) immobilized on N-doped carbon nanotubes (NCNT) for CO 2 RR are reported, which achieves the lowest onset overpotential of 16 mV for CO 2 -to-CO and the highest cathode energy efficiency of 86.9% with CO Faraday efficiency >99.0% to date. Interestingly, NiN x /NCNT affords a CO generation rate of 43.0 mol g −1 h −1 at a low potential of −0.572 V (vs RHE). DFT calculations reveal that the NiN x nanoclusters favor *COOH formation with lower Gibbs free energy than isolated Ni single-atom, hence lowering CO 2 RR overpotential. As NiN x /NCNT is applied to a membrane electrode assembly system coupled with oxygen evolution reaction, a cell voltage of only 2.13 V is required to reach 100 mA cm −2 , with total energy efficiency of 62.2%.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Yan Zhang,Chuang Chen,Qiu-Hui Zheng,Zhan-Kuo Guo,Bao-Xia Dong,Yun-Lei Teng
Metal heteroatom doped carbon materials display remarkable catalytic performance in the electrochemical CO2 reduction (ECR) because the doped heteroatoms can significantly change the local density of state and electronic structure of carbon, which induces charge polarization or structural defects. Herein, we synthesized S-doped NiII-triazolate precursors with high purity and crystallinity through a simple one-step hydrothermal method. The high-temperature pyrolysis process produced a series of Ni–S–CT (T = 800, 900, 1000 °C) materials with Ni3S2 as the main component. It resulted in significant carbon structure defects in the catalyst, which increased the specific surface area and pore volume, providing a basis for improving the ECR activity. Through the structural characterizations of powder X-ray diffraction (PXRD), Raman, X-ray photoelectron (XPS), Brunauer–Emmett–Teller (BET), transmission electron microscopy (TEM), and electrochemical characterizations of linear sweep voltammetry (LSV), chronoamperometry (i–t curve), electrochemical impedance spectroscopy (EIS), and electrochemical active surface area (ECSA), as well as gaseous product analysis, we can build the structural-performance relationship. Ni–S–CT catalysts all reached the highest CO Faraday efficiency at −1.5 V vs Ag/AgCl potential, among which Ni–S–C1000 exhibited the best catalytic activity (FECO of 66.6% and jCO of 1.28 mA/cm2). It also displayed excellent stability and recyclability, which could realize the efficient reuse of the catalyst. In addition, the density functional theory (DFT) calculation was carried out on Ni3S2 to illustrate the ECR activity origination. It is the first report on Ni3S2-based catalysts in the application of ECR.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Ye Wang,Yingkui Yan,Huabin Zhang,Xinsheng Peng,Hubiao Huang,Songtao Zhang,Li Shi
The development of unique single-atom catalysts with electron-rich feature is essential to promoting the photocatalytic CO 2 reduction, yet remains a big challenge. Here, a conceptionally new single-atom catalyst constructed from atomically dispersed Ni–P 3 species on black phosphorus (BP) nanosheets (BP-Ni) is synthesized for realizing highly efficient visible-light-driven CO 2 reduction when trapping photogenerated electrons from homogeneous light absorbers in the presence of triethanolamine as the sacrificial agent. Both the experimental and theoretical calculation data reveal that the Ni–P 3 species on BP nanosheets own the electron-rich feature that can improve the photogenerated charge separation efficiency and lower the activation barrier of CO 2 conversion. This unique feature makes BP-Ni exhibit the much higher activity as cocatalyst in the photocatalytic CO 2 reduction than BP nanosheets. The BP-Ni can also be applied as a cocatalyst for enhanced photocatalytic CO 2 reduction after combining with CdSe/S colloidal crystal photocatalyst. The present study offers valuable inspirations for the design and construction of effective catalytic sites toward photocatalytic CO 2 reduction reactions.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Dazhi Li,Rongfei Wang,Lingya Yi,Yunpeng Wei,Junying Li,Dantong Zhao,Wei Sun,Weihua Hu
It remains challenging to design alkaline hydrogen evolution reaction (HER) electrocatalyst able to stably operate at ampere-level current density . In this work, we successfully synthesized heterostructured Ni 3 S 2 /Cr 2 S 3 nanosheets on nickel foam (Ni 3 S 2 /Cr 2 S 3 /NF) for high current HER electrocatalysis in alkaline media . As-prepared Ni 3 S 2 /Cr 2 S 3 /NF reaches 0.5 and 1.0 A cm −2 currents at 230 and 333 mV overpotential, respectively. After 50 h test at 0.5 A cm −2 , the potential of Ni 3 S 2 /Cr 2 S 3 /NF remained almost unchanged. This impressive HER performance stems from its unique hybridization nature enabled hydrogen spillover, in which Cr 2 S 3 efficiently catalyzes the Volmer step, i.e., water dissociation to generate hydrogen, and the latter further transports to neighboring Ni 3 S 2 via spillover to facilitate the molecular hydrogen formation. This work provides a feasible strategy to synthesize efficient and durable HER catalysts for ampere-level water splitting.
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International Journal of Electrochemical Science
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2023
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IF 1.5
Huajing Zhu,Zeli Chen
Dye wastewater has the characteristics of high chroma, strong toxicity and difficult degradation, which has a serious impact on the environment. Because of its advantages of low energy consumption, simple operation and no secondary pollution, electrochemical oxidation technology has been increasingly studied in the field of refractory organic wastewater treatment. In this work, we report a multiwalled carbon nanotube (MWCNT)-MnO 2 nanocomposite as a Ni foam electrode modification. Then, the MWCNT-MnO 2 /Ni electrode is used for the electrochemical oxidation of Congo red dye. We study the effect of various factors on the decolorization of Congo red by the single-factor method. The results show that the decolorization rate of Congo red decreases with an increasing initial concentration and pH. In this work, hydroxyl radicals are detected by high-performance liquid chromatography. In the case of hydroxyl radicals and chloride ions acting separately, it is concluded that the indirect oxidation of chloride ions is the main mechanism during the process of electrocatalytic oxidation.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 36
·17186-17193
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IF 3.3
Yue Bai,Dongyang Shen,Guowang Yu,Jie Wang,Shuai Lyu,Yuhua Zhang,Guanghui Wang,Jinlin Li,Lin Li
The manufacture of high metal loading catalysts is of great interest in heterogeneous catalysis; however, there are challenges in the construction of the catalytic structure, including particle size, dispersion, and accessibility. Herein, we fabricate a high Ni loading catalyst by the carbonization–oxidation–reduction (COR) strategy for low-temperature dry reforming of methane. The carbon coating obtained by carbonizing organic ligands protects Ni nanoparticles from agglomeration and sintering. Subsequent oxidation–reduction treatment sacrifices carbon and causes Ni redispersion, resulting in dual particle size distribution. The sacrifice of carbon enhances the metal–support interaction and the resistance of metal sintering. 30% Ni/MCF-COR exhibits higher and more stable catalytic activity at relatively low reaction temperature compared with 30% Ni/MCF-H2. COR pretreatment is promising in the manufacture of high metal loading catalysts for the conversion of greenhouse gasses.
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International Journal of Electrochemical Science
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2023
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IF 1.5
Changshui Wang,Jiahui Zhang,Caiyan Shi,Dandan Cai
The development of an inexpensive, efficient and robust water oxidation catalyst is important to achieve water splitting for renewable energy production. Herein, nickel-cobalt layered double hydroxides (Ni-Co LDHs) were rationally synthesized by a facile method and can be served as efficient electrocatalysts for water oxidation. For comparison, Ni-Co LDH nanoflowers have also been synthesized by controlling the synthetic process. The composition and morphologies of the catalysts were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM) and X-ray photoelectron spectroscopy (XPS). The as-obtained Ni-Co LDH nanocages exhibit a high catalytic activity toward the water oxidation reaction (WOR). The electrochemical results show that the overpotential of Ni-Co LDH nanocages electrode was 350 mV at a catalytic current density of 10.0 mA cm -2 in 1.0 M KOH. Moreover, the Tafel slope was as low as ~ 93 mV dec -1 . The unusual catalytic properties of Ni-Co LDH nanocages could be attributed to the hollow structure and the synergetic effect between Ni metal and Co metal.
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International Journal of Electrochemical Science
·
2023
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IF 1.5
Yanni Shen,Xueli Miao,Dandan Song,Yanting Li,Yuning Qu,Jianguo Yu,Jiajun Tang,Hao Qin,Lili Wang,Jiahao Ren,Bing Wang
A facile and novel one-step hydrothermalmethod was provided for the preparation of Ni-Co double hydroxides (NC-DH), which was directly grown on carbonized cotton cloth (CCC) and used as advanced binder-free electrodes for supercapacitors. The effect of different concentration of Ni 2+ and Co 2+ in the intial reactant (C-Ni-x-Co-y) on microstructure and electrochemical performance were studied. The results showed that flake-like structure grown uniformly under an appropriate concentration, which was benefit to improve the electrochemical performance. The electrochemical tests revealed that the C-Ni-4-Co-8 electrode displayed the maximum specific capacitance of 4.19 F cm -2 when the current density was 5 mA cm-2and excellent rate capability maintained at 3.05 F cm -2 even at the high current density of 80 mA cm -2 . The electrodes of Ni-Co double hydroxides anchored on flexible conductive substrates with excellent electrochemical properties could be obtained by cost-effective method, which could be ascribed as a highly promising potential electrode material for energy storage devices.
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Catalysts
·
2023
·Vol. 13
·期 7
·1031
·
IF 3.9
Jie Lin,Yihong Ding,Huile Jin,Tianbiao Zeng
Nickel, cobalt, and manganese oxides are easily obtainable non-noble metal catalysts for water splitting. However, the relationship between composition and catalysts’ performance still needs systematic studies. Herein, guided by theoretical calculations, a low overpotential, easily prepared Mn-doped Co3O4was deposited on graphite plates for water splitting. The 30% Mn-doped Co3O4(Co2.1Mn0.9O4) required the lowest overpotential for oxygen evolution reaction (OER), in which the Co2.1Mn0.9O4reached 20, 30, and 50 mA cm−2in the overpotentials of 425, 451, and 487 mV, respectively, with 90% IR compensation. Under overall water-splitting conditions, the current density reached 30 mA cm−2at an overpotential of 0.78 V without IR compensation. Charge density difference analysis illustrates that doped Mn provides electrons for O atoms, and that Mn doping also promotes the electron fluctuation of Co atoms. XPS analysis reveals that Mn-doping increases the chemical valence of the Co atom, and that the doped Mn atom also exhibits higher chemical valence than the Mn of Mn3O4, which is advantageous to boost the form of based-OOH* radical, then decrease the overpotential. Considering the particular simplicity of growing the Co2.1Mn0.9O4on graphite plates, this work is expected to provide a feasible way to develop the high-performance Co-Mn bimetallic oxide for water splitting.Keywords:water splitting;bimetallic oxides;Mn-doped Co3O4;DFT calculation
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ACS Catalysis
·
2022
·
IF 13.7
Rui Ma,Junxian Gao,Jiajing Kou,David P. Dean,Christian J. Breckner,Kaijun Liang,Bo Zhou,Jeffrey T. Miller,Guojun Zou
Nickel has been considered a promising nonprecious metal for propane dehydrogenation (PDH) because of its appealing ability to activate alkane molecules; however, synthesis of selective and stable Ni sites remains a challenge. Herein, we describe an alumina-supported isolated Ni(II) site by settling Ni2+ cations into Al3+ vacancy on γ-Al2O3 as a selective and stable Ni-based catalyst for PDH. Based on the results from combined characterizations, including in situ X-ray adsorption spectroscopy (XAS), scanning transmission electron microscopy (STEM), and in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS), atomically dispersed Ni(II) sites with bonding to oxygen ions from the alumina support are demonstrated. PDH catalyst tests shows that the Ni(II) single-site catalyst delivers superior performance compared to a supported metallic Ni NP catalyst, possessing >93% propylene selectivity at considerable propane conversions (15–45%), which surpasses Ni nanoparticle (NP) catalysts. The correlation of selectivity to propylene on different Ni structures with the structural characterizations suggest that the coordinatively unsaturated tetrahedral Ni(II) sites facilitate the desorption of propylene, which inhibits the side reactions for coking. Moreover, the atomically dispersed Ni(II) sites remain in its local structure in the reaction-regeneration cycles, as evidenced by in situ XAS. This study on alumina-supported nickel catalysts affords insights into the nature of selective and stable nickel sites involved in the PDH reaction.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Jian Zhang,Yue Zhao,Maoxin Yang,Hong Jiang,Bing Wang,Yanping Jia,Weihua He
The abuse of doxycycline hydrochloride (DOX) in animal husbandry and its incomplete treatment have led to serious environmental problems, especially the risk of bacterial resistance. As an efficient, simple, and non-polluting method of catalysis, electrocatalysis has many advantages, which has attracted extensive attention in the removal of antibiotic pollutants in wastewater. Hence, the Ni/MWCNTs-OH/Ti composite electrode was prepared by galvanostatic electrodeposition to electrocatalyze DOX, and then the electrode was observed and analyzed by SEM , XRD and XPS. The optimal conditions (MWCNTs-OH was 0.10 mg/L, the concentration of NiSO 4 was 75 mmol/L, the degradation current was 15 mA, NaCl was present at a concentration of 0.20 mol/L, and pH value of 4) for degradation of 30 mg/L DOX within 60 min were determined by controlling variables. The degradation process of DOX followed Langmuir-Hinshelwood quasi-first-order reaction kinetics. As a result of stable the electrode, DOX removal rate was consistently above 70 % after 10 continuous uses, which showed good stability and reusability. The composite electrode electrocatalyzed DOX under the synergistic effect of cathode and anode. To identify the main intermediates involved in the electrochemical degradation of DOX, LC-MS was used. The toxicity of the intermediate products and final products was compared and analyzed by microbial culture experiment. And then Ecosar 2.2 was used to predict the biotoxicity of main intermediates to fish, daphnid, and green algae . This work provides a new material for the environmental remediation of antibiotic pollution.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Guoqiang Liu,Zhongti Sun,Dongming Liu,Yongtao Li,Weixin Zhang
Electrocatalytic urea oxidation (UOR) has attracted significant interest as a promising anodic half-reaction to replace sluggish oxygen evolution reaction (OER) toward water splitting. However, the activation and decomposition of urea molecule maintains a challenge during electrocatalytic process because of its 6e − oxidation procedure. Herein, Ni nanoparticles decorated NiMoO x nanorod (Ni/NiMoO x ) electrocatalyst with abundant heterojunction interfaces is fabricated and the density functional theory (DFT) calculation testifies that the interfaces are favorable for enhancing the conductivity and modulating the surface polarization of Ni/NiMoO x , thus improving its UOR’s activity. The Ni/NiMoO x performs superb electrocatalytic capacities toward UOR with a potential of 1.355 V ( vs RHE) at 20 mA cm −2 , and HER with an overpotential of 98 mV at 10 mA cm −2 . A hybrid two-electrode water splitting cell is further assembled via applying the Ni/NiMoO x as both anodic and cathodic electrodes with presence of 0.33 M urea, delivering 50 mA cm −2 at voltage of 1.589 V. The findings help to provide a reliable strategy for rational reconstruction of Ni based metal oxide with rich interfaces for diverse electrocatalytic reactions.
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