JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Xinzeng Zhang,Lixin Chen,Yuanyuan Liu,Jing Li,Meiri Wang,Hongtao Cui,Zhiwen Chen,Chandra Veer Singh,Kaihua Liu
Construction of heterogeneous interfaces with dual active components to synergistically promote both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is an effective strategy for facilitating electrochemical water splitting, but the appropriate active component regulation via simple synthesis procedures is still challenging. Herein, the Co and Co 2 Mo 3 O 8 active components are screened to construct effective heterogeneous interfaces and successfully integrated on Ni foam by thermal reduction of cobalt molybdate precursor. And this bifunctional electrode (Co/Co 2 Mo 3 O 8 /NF) required overpotentials of only 164 and 360 mV to drive the 100 mA cm −2 for HER and OER in alkaline media , respectively. Theoretical calculations showed that the electron transfer occurred from Co to Co 2 Mo 3 O 8 at the interface, then the formed interfacial cobalt atoms with deficient electron were beneficial for water activation, and reduced energy barrier of water dissociation under the synergistic effect of Co 2 Mo 3 O 8 . Notably, the alkaline electrolyzer based on symmetric Co/Co 2 Mo 3 O 8 /NF electrodes generated 100 mA cm −2 at a voltage of only 1.75 V, surpassing commercially available precious-metal Pt/RuO 2 -based catalysts.
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ChemistrySelect
·
2024
·Vol. 9
·期 15
·e202401460
·
IF 1.9
Wenting Chen,Shaoyi Li,Xue Lu,Jian Yang,Shaobo Cao,Kang Da,Ximei Fan
Graphical Hyperbranched phthalocyanine copper (HCuPc) wrapping nano-silica is synthesized via in situ polymerization and served as precursor for preparing atomically dispersed Cu−N−C electrocatalysts. Highly dispersed copper single-atom catalyst Cu-N−C has good electrocatalytic performance by using chemical anchoring of phthalocyanine and steric hindrance to restrict the migration and aggregation of Cu atoms. Atomically dispersed nonprecious metal-based catalysts have been considered as the most promising alternatives to Pt-based catalysts since their excellent catalytic activities and almost 100 % atom utilization in oxygen reduction reaction. However, the agglomeration of metal atoms is unavoidable during pyrolysis process, thus leads to the decrease of electrocatalytic performance. Herein, hyperbranched phthalocyanine copper (HCuPc) wrapping nano-silica is synthesized via in situ polymerization and served as precursor for preparing atomically dispersed Cu−N−C electrocatalysts. Owing to the confinement effect of chemical-anchoring and spatial-hindrance, the migration and agglomeration of Cu atoms are restricted in carbonization process. The aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray photoelectron spectroscopy (XPS) are performed to confirm the atomically dispersed of as-synthesized catalyst, which is labelled as HCu−N−C/SiO 2 . In addition, the HCu−N−C/SiO 2 possess superior ORR electrocatalytic activities with a half-wave potential of 0.874 V vs RHE and a limiting current density of 5.7 mA cm −2 . The zinc-air batteries assembled with HCu−N−C/SiO 2 catalyst exhibit a high specific capacity of 789 mAh g −1 as well as a maximum discharge power density of 176 mW cm −2 . This work proves that hyperbranched phthalocyanine structure could be a useful confined framework to the fabrication of singles-atom catalysts.
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Small
·
2025
·
IF 12.1
Ruiqi Guo,Shujuan Wang,Minqi Sheng,Xingli Zou,Mingzhi Zhang,Guangcheng Li,Yi Cao,Zhenglong Fan,Jinxin Chen,Wenxiang Zhu,Fan Liao,Tianjiao Ling,Hao Ren,Fan Lv,Zhenhui Kang
Iridium (Ir) is recognized to have extremely high catalytic activity in the hydrogen evolution reaction (HER). However, there are still technical challenges in maximizing the utilization of Ir atoms in the catalytic reaction process through dimensional regulation strategies. Herein, an innovative strategy is utilized to fabricate porous phosphorus-doped iridium (P-Ir) with a 2D structure, specifically the reduction of 1T phase-IrO 2 (1T-IrO 2 ) nanosheets using phosphine gas. The optimized P-Ir achieves an overpotential of 17.2 mV (vs RHE without i R-correction) in 0.5 m H 2 SO 4 during the HER process, outperforming benchmark Pt/C (27.0 mV) and most reported Ir-based electrocatalysts. During the long-term stability tests, P-Ir maintains stable operation for more than 100 h at both −10 and −100 mA cm −2 , respectively. Moreover, the HER activity and transient potential scanning results of Ir-based phosphides prove that doping P atoms in the Ir lattice promotes the reaction kinetic rate and charge transport capacity during hydrogen evolution. Theoretical calculations reveal that P atoms doping weakens the adsorption energy of H intermediates (H*) by regulating the d -band center of the Ir sites. Simultaneously, the desorption process of H* is also facilitated by forming a special bridged-H* bond structure, eventually accelerating the HER kinetics.
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Inorganic Chemistry Frontiers
·
2024
·Vol. 11
·期 6
·1852-1861
·
IF 6.1
Qihao Wu,Tao Xie,Li Zhang,Heju Gao,Jiahui Jiang,Ting Zhao,Guancheng Xu
Wearable and rechargeable zinc–air batteries (ZABs) hold significant potential for applications in flexible electronics and light weight power sources due to their high energy density and excellent safety. However, the practical use of ZABs is hindered by the slow kinetics of the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) on the air cathode. Here, we prepared S, N co-doped carbon nanotubes loaded with a cobalt–iron alloy (CoFe and Co0.72Fe0.28) and Co8FeS8 nanoparticles that can act as bifunctional electrocatalysts through one-step pyrolysis using the CoFe formic-acid framework (CoFe-FF) as the metal source. This electrocatalyst exhibited a superior electrocatalytic performance compared to commercial Pt/C (20 wt%) and RuO2. The ZAB assembled with CoFeS/SNCNT demonstrated an open-circuit voltage (OCV) of 1.47 V, a maximum power density (Pmax) of 175.3 mW cm−2, and a good cycle life. Furthermore, the flexible ZAB assembled with CoFeS/SNCNT achieved an OCV of 1.38 V and a Pmax of 77.7 mW cm−2, while maintaining stability under different bending angles. This study presents a feasible strategy for synthesizing and constructing high-performance non-noble metal bi-functional electrocatalysts for rechargeable zinc–air batteries.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Ruihong Guo,Yujuan Zhang,Xiutang Zhang,Hong Yang,Tuoping Hu
The use of the hydrazine oxidation reaction (HzOR) to replace the oxygen evolution reaction (OER), which has a large thermodynamic barrier and a slow kinetic process, is a feasible way to achieve energy saving hydrogen production, but the construction of superior bifunctional catalysts is also challenging. Herein, an array (CoFe 2 O 4 @NNWs) of CoFe 2 O 4 nanosheet grown in situ on nickel nanowires (NNWs) has been prepared and showed the excellent performance for hydrogen evolution reaction (HER) and HzOR under alkaline media, which require a lower potential of −91 mV (vs. RHE) for HzOR and 45 mV (vs. RHE) for HER at the current density (j, 10 mA cm −2 ). The overall hydrazine splitting (OHzS) electrolyzer requires cell voltages of 0.028 V (10 mA cm −2 ) and 1.227 V (1000 mA cm −2 ) by using electricity, wind, solar and thermal energies as power sources and had remarkable long-term stability. In addition, the potential of the OHzS is 1.67 V lower than that of OWS at the j of 10 mA cm −2 . The excellent performance of CoFe 2 O 4 @NNWs is attributed to the fact that the heterojunction fromed by CoFe 2 O 4 and NNWs effectively regulates the electron density of the sample, thereby improving the kinetics of H* adsorption and the N 2 H 4 dehydrogenation, which can be confirmed by DFT. Second, the continuous electron transport channel provided by NNWs improves the electrical conductivity of the sample. In addition, the 2D CoFe 2 O 4 nanosheets grown on NNWs not only expose more catalytic active sites, but also provide a fast channel for the diffusion of the electrolyte.
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GREEN CHEMISTRY
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2024
·Vol. 26
·期 4
·2011-2020
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IF 9.3
Lixia Wang,Xinran Hu,Huatong Li,Zhiyang Huang,Jia Huang,Tayirjan Taylor Isimjan,Xiulin Yang
Deliberate engineering of built-in electric fields (BEFs) can facilitate electron transfer and promote asymmetrical charge distribution, thereby regulating the adsorption/desorption of reaction intermediates. Herein, an oxygen-deficiency-rich MnO-CeO2 is synthetized supported on a carbon sphere (MnO-CeO2@Cs), adeptly crafted with a prominent work function difference (ΔΦ) and robust BEF, targeting the electrocatalytic oxygen reduction reaction (ORR). Empirical and theoretical results substantiate that the BEF triggers interfacial charge redistribution, fine-tuning the adsorption energy of oxygen intermediates and hastening reaction kinetics. Consequently, the MnO-CeO2@Cs showcases commendable performance (E1/2 = 0.80 V and jL = 5.5 mA cm−2), outshining its single-component counterparts. Impressively, the MnO-CeO2@Cs-based zinc–air batteries (ZABs) boast an exemplary power density of 202.7 mW cm−2 and enduring stability of 297 h. Additionally, the solid-state ZAB commands a peak power density of 67.4 mW cm−2, underscoring its potential in flexible ZAB applications. This work delineates a strategic avenue to harness interfacial charge redistribution, aiming to enhance the catalytic performance and longevity of energy conversion/storage apparatuses.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Ran Zhang,Yijiao Wang,Xinyu Gao,Donghong Duan,Junwen Wang,Shibin Liu
The theoretical potential of the urea oxidation reaction (UOR) is a mere 0.37 V(vs.RHE), significantly lower than the 1.23 V (vs. RHE) of the oxygen evolution reaction (OER). Thus, substituting the OER with the UOR can effectively reduce the voltage required for electrolysis. Transition metal phosphates (TM-Pi), with their unique physical properties, can partly replace precious metal catalysts and hold great application potential. However, further modification is necessary to enhance their catalytic activity and stability. Therefore, this study prepared a coral-like cluster Co/Zn-Pi@NF (Pi represents phosphate) catalyst, which was grown in situ on nickel foam (NF) using the constant current electrodeposition method. The catalyst exhibited superior catalytic performance in 1 M KOH, with the required overpotentials for the hydrogen evolution reaction (HER) and OER reaching 10 mA·cm −2 being 36.6 mV and 343.4 mV, respectively. In 1 M KOH containing 0.5 M urea, the urea oxidation potential was only 1.4 V, which remained stable for 60 hours. The Co/Zn-Pi@NF nanoparticles were used as the anode and cathode for water-urea electrolysis, and the electrolysis voltage was 1.43 V at a current density of 10 mA·cm −2 , which was 290 mV lower than that of electrolyzed water. This study demonstrates that zinc-cobalt bimetallic phosphate can be used as a dual-function electrocatalyst for hydrogen evolution and urea oxidation.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Ran Zhang,Xinyu Gao,Kaiyuan Zhang,Donghong Duan,Xianxian Zhou,Junwen Wang,Shibin Liu
In order to realize efficient hydrogen production with low energy consumption, the urea oxidation reaction (UOR) is the most practical alternative counter-reactions to the hydrogen evolution reaction (HER) in the overall electrochemical water splitting process. It’s highly desirable through the development of suitable cost-effective and non-precious catalysts, to design brilliant bifunctional electrocatalysts for the UOR and HER with both fast electron. Herein, the electrodeposition technique was used for synthesizing the hierarchical MnP/MnO@NiP on nickel foam (NF) and its electrocatalytic behavior was explored for HER and UOR. For delivering the 10 mA·cm −2 current density, the Co-MnP/MnO@NiP/NF electrode needed only 36.2 mV overpotential in HER and 1.24 V in UOR. During overall urea electrolysis, the cell voltage in 10 mA·cm −2 was only 1.52 V, which is 300 mV lower than the HER-OER process. The remarkable catalytic performance for HER and UOR can be attributed to the protective role of MnO x and the interfacial electron interactions within the material, which significantly boosted its overall activity, and the introduction of Co could enhance the electrochemical interface to obtain highly dispersed samples. The introduction of Ni could form a NiOOH with good catalytic activity intermediates with good catalytic activity to facilitate the UOR process.
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NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Jianzhi Wang,Hongyi Chen,Hongliang Yu,Wangshu Tang,Yuanhang Wu,Yijie Yang,Yu Luo,Jie Yang,Faquan Yu
Designing efficient and cost-effective nonprecious electrocatalysts for the hydrogen evolution reaction (HER) in alkaline solution still remains a significant challenge. Herein, we fabricated a three-dimensional (3D) transition bimetallic phosphate/reduced graphene oxide grown in situ on a nickel foam (NiCoP@rGO/NF) for the HER in alkaline media. NiCoP@rGO/NF exhibits a unique three-dimensional spherical nanostructure with a large specific surface area and short diffusion path, which are conducive to the transfer of electrons. NiCoP@rGO/NF requires an overpotential of only 94 mV at a current density of 10 mA cm−2, with a low Tafel slope (39 mV dec−1), and demonstrates excellent durability in 1.0 M KOH condition. Our work provides a new idea for designing high-performance HER electrocatalysts, which are highly needed in various practical applications.
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Molecular Catalysis
·
2024
·
IF 3.9
Jianwei Yuan,Kwame Nana Opoku,Pin Zhou,Jiaqing Cao,Yaorao Gao,Haoyang Peng,Baoliang Liu,Xiaohui Chen,Zhenwei Zhang,Fu Yang
The highly efficient green catalytic synthesis of jet fuel from low-chain biomass molecules is very attractive to afford sustainable development. Herein, ultrafine Ni nanoparticles assembled on Nb 2 O 5 nanofibers were constructed and effectively utilized in the reductive coupling of n-octanoic acid, offering a novel approach distinct from traditional hydrogenation methods for fatty acids. During the process, a synergistic effect was observed between the metallic Ni phase and the fibrous Nb 2 O 5 , facilitating immediate ketonization following reduction. This enabled the conversion of n-octanoic acid into pentadecane, a crucial component of aviation kerosene. The key factor driving this conversion was the attainment of a production rate of 8-pentadecanone higher than that of n-octane, particularly under optimal conditions, resulting in a significant yield of pentadecane. The catalytic assessment results show that adjusting Ni loading altered the performance of the catalyst in which 1.0 % Ni/Nb 2 O 5 afforded the best catalytic activity. By precisely controlling the reaction temperature at 300 °C and maintaining a hydrogen pressure of 1 MPa, an impressive pentadecane yield of 70.5 % was achieved. This innovative approach, which combines reduction with ketonization, offers a promising strategy for producing long-carbon chain alkanes from short-carbon chain fatty acids within a single reactor. This not only reduces economic costs but also streamlines overall processes, presenting a significant advancement in sustainable fuel production.
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FUEL
·
2024
·
IF 6.7
Taizhong Huang,Xuanhao Zhang,Xiaoming Zhou,Haizhou Zhang,Xiaochun Ma,Zhanyu Ding,Jiemei Yu
Nonprecious-metal-based materials show great potential to be highly efficient catalysts for oxygen reduction reaction (ORR). There is still room for improvement in the performances of nonprecious-metal-based catalysts for ORR. In this paper, we investigated the catalytic performances of N-doped carbon nanotubes (CNTs) with encapsulated cementite (Fe 3 C@CNT) for ORR. The encapsulation structure was confirmed by scanning electron microscopy, transmission electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy analyses. The catalytic performances of Fe 3 C@CNT for ORR were investigated by cyclic voltammetry, linear sweep voltammetry, Tafel analysis, rotating disk electrode, and rotating ring-disk electrode tests. The results showed that both the onset potential and half-wave potential of Fe 3 C@CNT-catalyzed ORR were 60 mV higher than those of 20 wt% Pt/C catalyst. Fe 3 C@CNT catalyzed ORR mainly happened through a four-electron pathway. The long-time running stability of the Fe 3 C@CNT was also superior to that of the 20 wt% Pt/C catalyst. The eutectic layers between the CNTs and cementite enhanced the electron transfer from the inner-layer CNT to the surface-layer N-doped CNT. Calculations revealed that the iron and carbon in the cementite were in positive and negative electronic states, respectively. The encapsulated cementite promoted the formation of equipotential circles on the surface-layer CNT, which greatly enhanced the catalytic performance of the Fe 3 C@CNT for ORR. N-doped CNTs with encapsulated cementite show great potential to be high-performance catalysts for ORR.
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Heliyon
·
2024
·
IF 3.4
Jun Dong,Qiqi Jiao,Hao Wang,Hong Wang,Yi-ke Ren
The shortcomings of precious metal based catalysts have limited the development of novel energies. So, developing low-cost and high performance transition metal based catalysts is one of the most feasible way to substitute the precious metal based catalysts. In all of the developed catalysts for oxygen reduction reactions (ORR), the iron-based nitrogen doped carbon nanotube (N-CNT) show great promise. In this paper, N-CNT with Fe 3 C encapsulated based catalysts (Fe 3 C@N-CNT) were synthesized. The encapsulation structure of Fe 3 C@N-CNT was confirmed by HAADF-STEM, XANES, XPS, XRD, SEM and other methods. XANES tests show that the doped nitrogen of Fe 3 C changed the length of Fe-C bond and furtherly influenced the electron transfer between encapsulated Fe 3 C and outer layer N-CNT. Electrochemical tests showed that the half-wave potential and onset potential ORR of 750 °C calcined Fe 3 C@N-CNT were 90 mV higher than that of 20 wt% Pt/C. The additional electric field between Fe 3 C and N-CNT modulated the C-N bond of surface N-CNT and enhanced the catalytic performance for ORR. This paper reveal that constructing encapsulated additional electron providing center is an effective way to design high performance catalysts.
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