Nanoscale
·
2022
·Vol. 14
·期 48
·17995-18002
·
IF 8.307
Lian-Hua Xu,Wen-Ju Wang,Xue-Ji Zhang,Serge Cosnier,Robert S. Marks,Dan Shan
Due to the complexity of the synthetic process of cobalt phosphides (CoP), ongoing efforts concentrate on simplifying the preparation process of CoP. In this work, amino tris(methylene phosphonic acid) (ATMP, L1) and melamine (MA, L2) are assembled into two-dimensional (2D) organic nanostructures by hydrogen bonding and ionic interactions via a supramolecular assembly, which greatly weakens the coordination ability of L1 with Co2+. As the introduced L2 is rich in carbon and nitrogen, it allows the cobalt–organophosphate complex to be placed under a strongly reducing atmosphere during the high-temperature calcination process to achieve an in situ phosphating purpose. The resulting catalyst (N-CoP/NC) exhibits the sought-after enhanced oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) performance. For the ORR in 0.1 M KOH, an enhanced onset potential (0.908 V vs. RHE) and diffusion limiting current (6.280 mA cm−2) can be obtained, which is comparable to those of 20% Pt/C (0.911 V vs. RHE, 5.380 mA cm−2). For the HER in 0.5 M H2SO4, an overpotential of 150 mV is required to drive a current of 10 mA cm−2. Moreover, Density Functional Theory (DFT) calculations reveal the catalytic pathway of N-CoP/NC.
研究领域:
材料科学
·
电催化
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Xinqi Han,Na Suo,Cheng Chen,Zihan Lin,Zhiyu Dou,Xingquan He,Lili Cui
It is accepted that the electrocatalytic activity is correlated to the morphology. Here, graphene oxide guiding nickel and iron layered double hydroxides hybrid arrays (GO-FeNi-LDH) are firstly fabricated by one-step electro-deposition method. The pretty 3D arrays with sheets vertically growing on nickel foam (NF) are highlighted by controlling the quantity of GO. Furthermore, the electron transfer from Ni, Fe to graphene is detected, making the metals and graphene in high valence and electron-rich state, respectively. The optimal GO-FeNi-LDH presents pretty morphology, defects, electron interactions and good conductivity. Therefore, to achieve 10 and 100 mA cm −2 , it requires the overpotentials of 119, 210, 285 and 303 mV for HER and OER and excellent durability. Noticeably, the optimal GO-NiFe-LDH needs a cell voltage of 1.48 V to drive 10 mA cm −2 for the whole water splitting, which are lower than that of most of advanced electrocatalysts , endowing it in first-rank electrocatalyst.
研究领域:
材料科学
·
电化学
·
纳米材料
·
能源化学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Aiping Li,Muhammad Shoaib,Hafeez Ur Rehman,Zhaotang Li
The oxygen evolution reaction (OER) hindered by its intrinsic sluggish kinetics remains a critical bottleneck in advancing water electrolysis and metal-air battery technologies. To address this challenge, herein, a Ru single-atom-anchored MoS 2 nanosheet array on carbon cloth (Ru–MoS 2 /CC) is rationally designed to regulate the local electronic structure at the atomic scale. The isolated Ru atoms induce substantial electronic reconstruction of the MoS 2 matrix, manifested by charge redistribution, work-function reduction, enhanced electronic states near the Fermi level, orbital hybridization, and optimized d -band configuration. Such synergistic electronic modulation effectively tailors the adsorption energetics of key HER/OER intermediates (H* and OOH*), leading to markedly improved bifunctional electrocatalytic activity. Consequently, the optimized Ru-MoS 2 /CC delivers low overpotentials of 230 mV at 50 mA‧ cm −2 for OER and 103 mV at 10 mA‧ cm −2 for HER in 1 M KOH. This work highlights atomic-scale electronic engineering as an effective strategy for developing high-performance MoS 2 -based bifunctional electrocatalysts and provides fundamental insights into structure–activity relationships for sustainable water electrolysis.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xue Liu,Wei Yan,Jie Song,Hao Song,Wenmiao Chen,Yuexing Zhang,Yanli Chen
Enhancing the exposure of active sites and optimizing the electronic structure of the catalysts are indispensable for efficient catalyst design, yet remains challenging in the renewable energy field. Herein, a sequential pyrolyzing and phosphating approach for a well-designed GO/CoTPP gel precursor has been explored to prepare a Co-based carbon catalyst containing single-atom Co-N x and hollow Co 2 P active species (Co 2 P/Co-N-C) for multifunctional electrocatalytic reactions. Kirkendall effect occurring during the template-free one-pot phosphating approach induced the formation of the hollow Co 2 P structure in the catalyst, simultaneously optimizing the electron structure and allowing the active sites to be exposed to a greater extent. DFT calculations demonstrated that the Co 2 P and Co-N x structures enable Co 2 P/Co-N-C to have a suitable d-band center depending on the electron transfer from Co 2 P to Co-N x , which enhances the adsorption of O* and the dissociation of OH* in oxygen electrode reactions, thereby facilitates catalytic reactions. As a result, the Co 2 P/Co-N-C exhibits excellent trifunctional activity with a half-wave potential of 0.89 V in alkaline for oxygen reduction reaction (ORR), overpotentials of 330 mV for oxygen evolution reaction (OER) and 190 mV for hydrogen evolution reaction (HER), respectively, which are among the best results reported to date for Co-containing carbon-based catalysts. Furthermore, the flexible Zinc-air battery with Co 2 P/Co-N-C electrodes also demonstrates a high open circuit voltage of 1.35 V, which is applied to build the self-powered device for water splitting continuously. Our work provides a facile strategy to prepare high-performance trifunctional catalysts by morphology/structure control of metal-based NPs on carbon-based materials.
研究领域:
材料科学
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电化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Xinqi Han,Zihan Lin,Xingquan He,Lili Cui,Dongxiao Lu
Here, Fe, Co-layered double hydroxide and polyaniline composites onto nickel foam (NF) (FeCo-LDH/PANI) were fabricated via one-step co-electrodeposition method. The test results indicate the co-existence of the amorphous structure and the smaller size of crystal district with more defects in optimal FeCo-LDH/PANI. Importantly, it is found that there are more defects in FeCo-LDH/PANI compared to that of FeCo-LDH possibly attributed to the local etching of H + released from the polymerization of aniline. Benefitting from the numerous defects, higher electrochemical surface area (ECSA), lower charge-transfer resistance and electron interaction, the optimized FeCo-LDH/PANI needs the overpotentials of 104, 246, 285 and 323 mV vs RHE for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) to achieve 10 and 100 mA cm −2 , and shows desirable stability. Noticeably, the optimal FeCo-LDH/PANI requires a cell voltage of 1.53 V to drive 10 mA cm −2 for the whole water splitting.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Hao Zhang,Guang Yang,Yan Sun,Shirong Kang,Mingyu Dou,Hua Yang,Dacheng Li,Jianmin Dou
A heterocycle 2,5-bis(2-pyridyl)-1,3,4-thiadiazole (bptd) as a polydentate reacts with CoCl 2 ∙6H 2 O and NiCl 2 · 6H 2 O to form two novel monomeric complexes, [Co(bptd) 2 Cl 2 ]∙4H 2 O ( 1 ) and [Ni(bptd) 2 Cl 2 ]∙4H 2 O ( 2 ). The complex 1 can act as electron cocatalyst to improve the rate of hydrogen evolution of CdS NRs under visible light irradiation . After the introduction of cobalt lactate complex as a hole cocatalyst, this noble-metal-free system exhibited a hydrogen evolution rate of 1123 μmol h −1 , which is 12.2 times higher than that of pure CdS NRs. This system could work for 50 h with a TON of 7490, and the average AQY is 17% at 420 nm. Based on the results of experiments, the synergistic effect of complex 1 and cobalt lactate complex is proved and a possible mechanism for hydrogen production is proposed. This work may provide a reference for remedying the defects of faster carrier recombination and photocorrosion of CdS in heterogeneous environment.
研究领域:
材料科学
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催化
·
光化学
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纳米技术
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
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
·
材料科学
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催化
·
能源材料
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiaoe Dang,Sining Yun,Yongwei Zhang,Jingjing Yang,Zhuolei Liu,Changwei Dang,Yinhao Wang,Yingying Deng
With the increasing energy demands and impending climate change, significant concerns have been raised over the metal–organic frameworks (MOFs)-derived porous carbons and their utilization for hydrogen evolution reaction (HER) and triiodide reduction reaction (IRR). However, the provision of high intrinsic activity, active-site accessibility, and structural stability of MOF-derived Co-embedded N-doped carbon (Co/N-C) for HER and IRR is challenging. In this work, core-shell MOF-in-MOF precursors are designed to construct novel double-shell N-C-in-Co/N-C electrocatalysts with nanorod- and rhombic dodecahedron-shaped hollow morphologies (NR-H-C and RD-H-C). The double-shell structured NR-H-C and RD-H-C significantly enhance the HER and IRR activity of Co-MOF-derived Co/N-C. Specifically, NR-H-C achieves a high N-content (10.35 at.%), large specific surface area (590.87 m 2 g −1 ), and hierarchical porous configuration (micropores and mesopores). When NR-H-C is applied as the HER catalyst in alkaline electrolyte, it exhibits an admired overpotential of 123 mV at 10 mA cm −2 and a Tafel slope of 51 mV dec −1 . The solar cell adopting NR-H-C as counter electrode for IRR achieves a high short circuit current density of 16.77 mA cm −2 , an open-circuit voltage of 0.745 V, a fill factor of 0.682, and a power conversion efficiency of 8.51%, higher than that of Pt-based solar cell (16.26 mA cm −2 , 0.744 V, 0.602, and 7.28%). The elucidatory Volmer-Heyrovsky HER mechanism and reversed Volmer-Heyrovsky IRR mechanism give a better understanding of the enhanced dual-functional activity of NR-H-C. This work provides an essential information for the rational design of high-performance dual-functional HER and IRR catalysts and further open up a new avenue for the construction of multicomponent MOFs in the energy conversion field.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 19
·10635-10644
·
IF 3.049
Xiaoxu Xuan,Jun Cheng,Xiao Yang,Junhu Zhou,Kefa Cen
Carbon supported nano-metal catalysts are expected to improve CO2 reduction selectivity and efficiency due to the addition of more active sites and enhancement of electron transport ability. In this study, HKUST-1 was pyrolyzed and decorated with Pt to prepare Pt–Cu/C catalysts. The catalytic effect of the catalysts with different Pt contents in the CO2 photoeletrochemical reduction reaction (CO2PRR) were compared. The total carbon atom conversion rate in CO2PRR experiments using Pt–Cu/C catalysts first increased to a peak when using 1.6 wt% Pt–Cu/C catalyst and then decreased with the increase of Pt content. The 1.6 wt% Pt–Cu/C catalyst showed good hydrogen evolution reaction (HER) inhibiting ability compared with other Pt–Cu/C catalysts. Density functional theory (DFT) calculations were conducted to give an insight into the CO2PRR mechanism on some possible active sites in Pt–Cu/C catalysts. The result demonstrated that HER was more likely to be inhibited on the Cu/Pt active surface and at the same time CO2PRR was promoted.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Shuli Yin,Songliang Liu,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Thermodynamically favorable oxidation reaction instead of oxygen evolution reaction (OER) with sluggish kinetics as anode reaction and coupled with hydrogen evolution reaction (HER) at cathode is an effective hydrogen production technology . Herein, we report a solvothermal method synthesis of defect-rich crimped perforated PdIn bimetallene as an efficient catalyst for hydrogen production with the assistance of methanol. Boosted by abundant crystal defects , higher surface energy and expanded surface active sites, the defect-rich crimped perforated PdIn bimetallene exhibits superior activity and stability in catalyzing methanol oxidation reaction (MOR) and HER. At the established MOR-HER co-electrolytic system, when the anode and cathode are equipped with PdIn bimetallene, the required cell voltage only is 1.26 V to achieve the current density of 100 mA cm −2 , which is 0.93 V lower than that of traditional water electrolysis. This work reports a defect-rich crimped perforated PdIn bimetallene catalyst, as an effective bifunctional catalyst that provides insight for the advancement of energy-saving and promising hydrogen production engineering.
研究领域:
催化
·
氢能
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Sustainable Energy & Fuels
·
2023
·Vol. 7
·期 13
·3116-3121
·
IF 5.6
Xinyue Wang,Yibin Wang,Xinzhi Ma,Lingling Xu,Sirui Liu,Wei Wang,Huiqing Lu,Lili Wu
Cobalt diselenide (CoSe2) is considered a promising catalyst for hydrogen evolution reaction (HER); however, the limited active number, agglomeration, and quick deactivation by acid etching hinder its broad adoption. Herein, we report carbon layer-covered CoSe2 nanowire arrays grown on carbon cloth (C@CoSe2/CC). The structure of the nanowire array demonstrates synergistic effects in promoting the infiltration of electrolytes, accelerating the diffusion of H2 bubbles, and preventing CoSe2 from being etched by the electrolyte. Consequently, the overpotential and Tafel slope (193 mV, 54.3 mV dec−1) obtained sustained 24 h with a negligible overpotential deterioration. This study provides insights into optimizing the intrinsic activity of active sites.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
TRANSITION METAL CHEMISTRY
·
2023
·Vol. 48
·期 2
·125-133
·
IF 1.7
Hu Yi,Xu Jingsong,Zhang Tianzhu,Zhong Hang,Chen Jun,Liu Xinai,Pan Qifa,Liu Ruidong,Jiang Chunli,Chen Jun
Electrocatalytic water splitting to produce hydrogen is a promising route to provide green hydrogen on a large scale. To explore non-noble metal electrocatalysts with high performance is still a challenge. Herein, a one-step electrodeposition way is developed to construct the heterostructural (NiO-La 2 O 3 )/(Ni-La)/NiO/Ni electrocatalysts on Ni foam. The dark Ni-La coating was prepared by co-electrodeposition from an aqueous solution containing LaCl 3 and NiCl 2 with a molar concentration ratio of 1:5. Among these heterostructural Ni-based electrocatalysts, an excellent HER activity is achieved: an overpotential of 22 mV at the current density of 10 mA cm −2 in 1 M KOH solution. It is demonstrated that the introduction of La significantly reduces the overpotential for HER. The higher the La content in the Ni-La coating of these electrocatalysts, the better the electrocatalytic HER performance was exhibited. This work provides a facile and inexpensive route to prepare Ni-La coating on electrodes in an aqueous solution.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）