SOLID STATE SCIENCES
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2022
·
IF 3.752
Shijun Xu,Yi He,Siming Yan,Teng He,Hongjie Li,Xiao Guo,Yi Fan
Hydrogen energy is the most promising clean energy at present and hydrogen production by electrocatalytic water splitting is the frontier technology of alternative energy in the future. Herein, the Ni–Mo alloy supported with nickel foam (NF) was prepared by hydrogen reduction strategy at high temperature. The catalytic activity and stability of NiMo@NF-x catalyst (x stands for temperature) with multistage (sheet/particle) array structure were studied under different temperatures. The performance of the catalyst was evaluated by contact angle and related electrochemical characterization. It was found that the surface of NiMo@NF-550 catalyst prepared at 550 °C had superhydrophilic and superaerophobic properties, which contributed to the deactivation of bubbles from the surface of the electrode and improved the efficiency of the catalytic reaction. Moreover, the multi-stage array structure of sheet/particle will form a greater specific surface area than the plain sheet structure, offering more reaction sites. These results indicate that the self-supported superhydrophilic and superaerophobic Ni–Mo catalysts have excellent electrocatalytic hydrogen evolution ability.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Jiaxian Liu,Xinyu Fan,Guyang Ning,Man Zheng,Kun Shi,Yuena Sun,Yongjun Gao,Yufan Zhang,Huan Wang
High-efficiency and economical electrocatalysts for electrochemical water splitting are the core component of the renewable energy conversion. Herein, a simple and economical strategy is described to synthesize a series of metal oxide decorated nitrogen-doped carbon nanotubes materials (N-CNT@Cu–Fe Oxide Alloy NPs) by utilizing carbon nanotubes as the substrate carrier material. Additionally, the polypyrrole (PPy) was served as both the nitrogen resource and the localizing agent to load the Cu–Fe oxide alloy. Moreover, the theoretical and test results indicated that the superior HER and ORR performance is mainly related to the synergistic effect between the nitrogen-doped CNT and metallic oxide alloy. In the series of catalysts we prepared, N-CNT@Cu 1 –Fe 1 Oxide Alloy NPs exhibits more significant catalytic activity and better durability than other catalysts that we synthesized. Meanwhile, the catalyst shows the low Tafel slope of 68.28 mV dec −1 for HER and reaches 10 mA cm −2 at the overpotential of 375 mV. The K–L plot shows that the electron transfer number of N–CNF@Cu 1 –Fe 1 Alloy NPs is 3.43.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Shaopei Jia,Yifan Cheng,Quan Huang,Qisong Li,Qian Zhang,Zhixin Wang,Yan Zhang,Niu Zhang,Yunchao Mu
Developing inexpensive and efficient electrocatalysts for hydrogen evolution reaction (HER) in both acidic and alkaline mediums is of great significance to the hydrogen energy industry. Hereby, we prepared a mixture of precursors with homogeneous composition by using the chelating ability of soybean protein isolate (C and N source) and phytic acid (dopant and phosphating agent) with cobalt ions , and achieved one-step synthesis and construction of Co 2 P/N–P co-doped porous carbon composite by carbonization at 800 °C. The as-synthesized Co 2 P/NPPC-800 electrocatalyst exhibits low HER overpotentials of 121 and 125 mV at 10 mA cm −2 in 0.5 M H 2 SO 4 and 1.0 M KOH, which are close to those of the commercial Pt/C catalyst. Additionally, the NPPC substrate surrounding the Co 2 P could diminish the corrosion during the HER, and Co 2 P/NPPC-800 displays good stability and durability. Furthermore, this work offers a convenient synthesis strategy for phosphide/doped porous carbon composites in other electrochemical energy technologies.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Xinkuai He,Zhousi Hu,Ruqing Guo,Yiren Li,Luye Wu
One of the most critical challenges in the field of hydrogen production through water electrolysis technique is the design, development and manufacture of electrode materials with low-cost, highly electrocatalytic activity and stability. We employ the galvanostatic deposition technique to prepare the honeycomb structured Co−Ni−Mo alloy electrocatalysts from ethylene glycol (EG) system, in which the honeycomb structure presents highly intrinsic electrocatalytic activity for hydrogen evolution reaction (HER). The electrochemical behavior of Co 2+ , Ni 2+ and Mo 6+ reductions and the co-deposition behavior of Co-Ni, Co-Mo, Ni-Mo and Co-Ni-Mo alloys is reported. Benefiting from the composition engineering by alloying with Mo atoms, as well as the simultaneous existence of a suitable honeycomb structure, these Co 58 Ni 23 Mo 19 deposits obtained at an optimal parameter exhibit prominent electrocatalytic durability and activity with a η 10 of 51 mV for HER in a 1.0 M KOH. More importantly, the formation model of the honeycomb structured Co-Ni-Mo alloy deposits is proposed. This work suggests a simple and economical method for the preparation of a 3-dimensional catalytic electrode.
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高影响因子
Nanoscale
·
2023
·Vol. 15
·期 48
·19784-19791
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IF 6.7
Xu Yang,Mengxue Liu,Fang Cui,Qinghai Ma,Tieyu Cui
Research on Ni/NiO electrocatalysts has advanced significantly, but the main obstacles to their use and commercialization remain their relatively ordinary activity and stability. In this paper, a chelating structure based on the coordination of multidentate ligands and Ni(II) is proposed to limit the growth of Ni and Ni oxide grains. These features reduce the particle size of Ni/NiO, increase particle dispersion, and maintain the high activity and stability of the catalyst. Aspartic acid, as a polydentate ligand, could coordinate with Ni2+ to form structurally stable chelate rings. The latter can limit grain growth, but also coat the active core with thin carbon layers after calcination to further achieve the confinement and protection of nanoparticles. The hydrogen evolution overpotential of prepared nitrogen-doped graphitized carbon shells (Ni/NiO@NC) nanoparticles was 100 mV (vs. RHE) when the current density was 10 mA cm−2 in 1 M KOH. The hydrogen evolution overpotential increased by only 4 mV after 6000 continuous cyclic-voltammetry scans. Moreover, when coated on different conductive substrates, the overpotential of this catalyst dropped to 34.6 mV (vs. RHE) at a current density of 10 mV cm−2. The lowest overpotential of the composite was only 194.9 mV at a current density of 100 mA cm−2, which is comparable with that of noble metal-based electrocatalysts. This work provides a plausible method for designing high-performance electrocatalysts of small size.
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高影响因子
VACUUM
·
2018
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IF 2.067
Ruifeng Liu,Wenxian Wang,Hongsheng Chen,Minbo Tan,Yuyang Zhang
With the advantage of micro-size and nano-size B 4 C particles, micro-/nano-bimodal size B 4 C particles have been widely used to fabricate excellent composites with high strength and ductility. In this study, micro-/nano-bimodal size B 4 C particles reinforced aluminum matrix composites with three different volume fractions (3%, 5% and 7%) were fabricated by spark plasma sintering (SPS) followed by hot extrusion and rolling (HER). The microstructure evolution and mechanical properties of as-SPSed, as-extruded and as-rolled composites were investigated. Results show that the microscopic electrical discharge between the particles in SPS promotes the densification of composites. The maximum relative density of as-SPSed composites increases from 99.21% to 99.65% after HER. Nano-size B 4 C particles distribute mainly at the gap of 6061Al particles in as-SPSed composites, while the microstructure presents more homogeneous after HER. Pin effect of nano-size B 4 C particles stimulates dynamic recrystallization (DRX) and grain refining. Texture orientation of the 6061Al grain exists in the as-extruded and as-rolled B 4 C/6061Al NCs. No new phases are detected in composites in all deformation stages. The tensile strength of as-SPSed composites increases when compared with 6061Al matrix, and the tensile strength of as-rolled composites after hot extrusion is enhanced to 305 MPa. Fracture mechanisms of as-extruded and as-rolled composites mainly include 6061Al matrix tear, particle/matrix interfacial tear and micro-size B 4 C particle fracture.
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ChemSusChem
·
2024
·
IF 7.5
Lina Jia,Gaohui Du,Di Han,Yunting Wang,Youqing Wang,Huayu Li,Wenqi Zhao,Shixian Chen,Miao Zhang,Qingmei Su,Bingshe Xu
Graphical P-doped NiFe 2 O 4 nanoparticles/N-doped carbon nanotubes are prepared via a hydrothermal method followed by phosphorization. The CNTs greatly enhance the electron transfer rate and the P-doping effectively modulates the charge distribution around Ni and Fe atoms, optimizes the energy barriers of adsorption of intermediates, urea and water dissociation, thereby accelerating the kinetics of water splitting and urea electrolysis. The design and construction of highly efficient electrocatalysts for overall water splitting and urea electrolysis are significantly important for promoting energy conversion and realizing green hydrogen production. In this work, we constructed a multi-phase heterojunction through a simple hydrothermal and phosphorization process. The P-doped NiFe 2 O 4 (P-NiFe 2 O 4 ) nanoparticles were uniformly anchored on the bamboo-like N-doped carbon nanotubes (NCNTs) grown via a NiFe-alloy autocatalysis. The electronic structure and coordination environment of active species were optimized by the synergistic action of P doping, well-dispersed ultrafine NiFe 2 O 4 , and NCNTs matrix with good conductivity, enhancing their quantity and activity for electrocatalysis. Consequently, the P-NiFe 2 O 4 /NCNTs/NiFe exhibits excellent HER and OER activities with an overpotential of 111 and 266 mV at 10 mA cm −2 in 1 M KOH, respectively. The symmetrical overall water-splitting cell using P-NiFe 2 O 4 /NCNTs/NiFe as both anode and cathode delivers 10 mA cm −2 at a voltage of 1.604 V in 1 M KOH. Notably, the two-electrode cell requires a low voltage of 1.467 V to achieve a current density of 10 mA cm − 2 in 1 M KOH solution with 0.6 M urea. This designed catalysts display outstanding reaction kinetics and catalytic stability. This work provides useful guidance for applying transition metal-based catalysts for hydrogen production.
研究领域:
材料科学
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电化学
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催化
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能源转换
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氢气生产
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Small
·
2024
·
IF 13
Yingyan Ma,Yuan Ha,Liangqiang Chen,Ziqi An,Linzhuang Xing,Zhenni Wang,Zhimin Li
Efficient and affordable price bifunctional electrocatalysts based on transition metal oxides for oxygen and hydrogen evolution reactions have a balanced efficiency, but it remains a significant challenge to control their activity and durability. Herein, a trace Ru (0.74 wt.%) decorated ultrathin CoOOH nanosheets (≈4 nm) supported on the surface of nickel foam (Ru/CoOOH@NF) is rationally designed via an electrochemically induced strategy to effectively drive the electrolysis of alkaline overall water splitting. The as-synthesized Ru/CoOOH@NF electrocatalysts integrate the advantages of a large number of different HER (Ru nanoclusters) and OER (CoOOH nanosheets) active sites as well as strong in-suit structure stability, thereby exhibiting exceptional catalytic activity. In particular, the ultra-low overpotential of the HER (36 mV) and the OER (264 mV) are implemented to achieve 10 mA cm −2 . Experimental and theoretical calculations also reveal that Ru/CoOOH@NF possesses high intrinsic conductivity, which facilitates electron release from H 2 O and H-OH bond breakage and accelerates electron/mass transfer by regulating the charge distribution. This work provides a new avenue for the rational design of low-cost and high-activity bifunctional electrocatalysts for large-scale water-splitting technology and expects to help contribute to the creation of various hybrid electrocatalysts.
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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能源转换与存储
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Materials Today Chemistry
·
2026
·
IF 7.4
Chunyan Fan,Zehao Zang,Yao Tang,Yahui Cheng,Lanlan Li,Xiaofei Yu,Xiaojing Yang,Zunming Lu,Xinghua Zhang,Hui Liu
Bifunctional N,P-codoped Ag catalyst achieves outstanding seawater electrolysis performance. • Enhanced HER via optimized H adsorption and H–H coupling enabled by N,P codoping. • In situ generated PO 4 3− activates lattice oxygen, lowers OER barrier, suppresses Cl − adsorption. Herein, we present a bifunctional N,P-co-doped Ag (N,P–Ag) catalyst synthesized via one-step electrodeposition for efficient alkaline seawater splitting. The catalyst achieves low overpotentials of 260 mV@50 mA cm −2 for oxygen evolution reaction (OER) and 49 mV@10 mA cm −2 for hydrogen evolution reaction (HER), along with excellent reaction kinetics and long-term stability (sustained operation for 200 h at 100 mA cm −2 ). DFT calculations disclose that N, P co-doping enhances HER activity by disrupting Ag's electronic configuration to create new hybrid orbitals and delocalized electronic states, which in turn optimize H* adsorption and accelerate H–H bond formation. In-situ Raman spectroscopy captures the surface restructuring process during OER that leads to the formation of the active phase PO 4 3- -AgO. The lattice oxygen-mediated mechanism (LOM) enables lattice oxygen to participate directly in the OER process, helping to optimize the energy levels of intermediate reactions and weaken Cl − adsorption, thereby effectively suppressing chloride ion corrosion. This work demonstrates a combined approach of non-metallic doping for electronic tuning and in-situ anion modification for lattice oxygen activation, providing a viable route to achieve efficient and corrosion-resistant seawater electrolysis. By modulating electron conduction via N/P doping, localized charge enrichment zones are created around Ag atoms as HER-active sites, while in situ-generated PO 4 3− activates lattice oxygen, lowering the reaction barrier and inhibiting chloride corrosion. Download: Download high-res image (357KB) Download: Download full-size image
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GREEN CHEMISTRY
·
2025
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IF 9.2
Yating Hou,Xiaoli Sun,Shan Lu,Ningyuan Song,Yanru Liu,Shu Yang,Fangxu Dai,Yunmei Du,Lei Wang
It is a challenge to enable non-precious metal-based electrodes to exceed the ultra-high alkaline HER activity of Pt-based precious metals by constructing a ‘vacancy–dopant structure’ with controllable vacancy concentration. Density functional theory (DFT) calculations revealed that the ‘P vacancy (Pv)–Cr dopant structure’ stimulates a significant enhancement-tandem effect during the alkaline HER process. This enhancement effect is reflected in enhanced conductivity and the adsorption capability of H2O and OH*, thereby reducing the reaction energy barrier. Simultaneously, the tandem effect induces the Cr dopant near Pv as a unique OH* adsorption site, thereby activating the Ni(Pv)–P–Cr(Pv) mechanism that effectively prevents the poisoning of Ni hydrophilic sites and optimizes the alkaline HER pathway. Based on these findings, Cr–NiPv/IF with the ‘Pv–Cr dopant structure’ was innovatively constructed using the ‘phosphorization-quenching’ technique. Interestingly, the quenching temperature difference is positively correlated with the Pv concentration. Under the enhancement-tandem effect of the ‘Pv–Cr dopant composite structure’, Cr–NiPv/IF only requires 240 mV to deliver 1 A cm−2 for alkaline HER, which is 3.04-fold higher than that of Pt/C@IF. This work offers a novel design concept for constructing non-precious metal-based electrodes that surpass the performance of Pt-based electrodes.
研究领域:
电催化
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材料科学
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析氢反应
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密度泛函理论
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纳米材料
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高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 40
·15446-15457
·
IF 4.569
Siyu Dai,Yuqi Liu,Yunjie Mei,Jue Hu,Kaiming Wang,Yanghua Li,Nanhao Jin,Xinying Wang,Huilong Luo,Wei Li
A novel two-dimensional Co-MOF material {[Co(dptz)2(oba)2]·(DMF)2}n is prepared using mixed organic ligands, which exhibits both OER (oxygen evolution reaction) and HER (hydrogen evolution reaction) catalytic performance. The integration of an Fe dopant and amorphous interface into Co-MOF to improving the electrocatalytic performance of pristine MOFs (metal–organic frameworks) is demonstrated and the origin of the remarkable electrocatalytic performance of the catalyst is elucidated. The comprehensive characterization data of Fe@Co-MOFs illustrate that there is a crystallinity transition during the doping of Co-MOF, which increases the electron transfer rate of the material and ensures increased exposure of the ligand unsaturated active site on the surface, and modulates the electronic structure of the Co center in a synergistic manner. As a result, the optimized catalytic Fe@Co-MOF-3 with an amorphous structure exhibits outstanding electrocatalytic performance for the OER, with only 248 mV at a current density of 50 mA cm−2 and excellent stability after 11 h of testing in alkaline solution. Not only that, the HER was achieved with a low overpotential of 150 mV at 10 mA cm−2. The present work indicates that the as-synthesized Co-MOF and Fe@Co-MOFs offer prospects in developing electrocatalysts for water splitting.
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Green Energy & Environment
·
2024
·
IF 10.7
Yingchun Niu,Yinping Liu,Tianhang Zhou,Chao Guo,Guangfu Wu,Wenjie Lv,Ali Heydari,Bo Peng,Chunming Xu,Quan Xu
Iron-chromium flow batteries (ICRFBs) have emerged as an ideal large-scale energy storage device with broad application prospects in recent years. Enhancement of the Cr 3+ /Cr 2+ redox reaction activity and inhibition of the hydrogen evolution side reaction (HER) are essential for the development of ICRFBs and require a novel catalyst design. However, elucidating the underlying mechanisms for modulating catalyst behaviors remains an unresolved challenge. Here, we show a novel precisely controlled preparation of a novel thermal-treated carbon cloth electrode with a uniform deposit of low-cost indium catalyst particles. The density functional theory analysis reveals the In catalyst has a significant adsorption effect on the reactants and improves the redox reaction activity of Cr 3+ /Cr 2+ . Moreover, H + is more easily absorbed on the surface of the catalyst with a high migration energy barrier, thereby inhibiting the occurrence of HER. The assembled ICRFBs have an average energy efficiency of 83.91% at 140 mA/cm 2 , and this method minimizes the electrodeposition process and cleans the last obstacle for industry long cycle operation requirements. The ICRFBs exhibit exceptional long-term stability with an energy efficiency decay rate of 0.011% per cycle at 1000 cycles, the lowest ICRFBs reported so far. Therefore, this study provides a promising strategy for developing ICRFBs with low costs and long cycle life.
研究领域:
能源存储
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催化
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电化学
·
材料科学
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