APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yujia Zhang,Kunkun Nie,Binjie Li,Lixin Yi,Chen Hu,Ziyi Wang,Xiaorong Hao,Wenlin Zhang,Zhengqing Liu,Wei Huang
The incorporation of rare earth (RE) elements into high-entropy alloys (HEAs) as electrocatalysts for hydrogen evolution reaction (HER) shows great potential in addressing the energy crisis. Here, we successfully synthesized cerium (Ce)-tailored PdCeMoCuRu HEA with chemical homogeneity and stability using a facile wet-chemical synthesis strategy. The obtained PdCeMoCuRu HEA provides abundant active metal sites, resulting in superior HER performance compared to state-of-the-art Pt/C. It only requires 12.8 mV to achieve a current density of 10 mA cm −2 , which is nearly half that required for Pt/C (24.8 mV). Importantly, it exhibits excellent electrocatalytic durability for 100 hours even under a high current density of 1.0 A cm −2 at the ampere level. Density functional theory (DFT) calculations confirm that the introduction of Ce can modify the electronic configuration and generate synergistic effects around Pd, Cu, and Ru active sites. This work establishes a novel approach for designing efficient RE-tailored HEA electrocatalysts.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2015
·
IF 4.642
Shanlong Chen,Aichun Xu,Jie Tao,Haijun Tao,Yizhou Shen,Lumin Zhu,Jiajia Jiang,Tao Wang,Lei Pan
A novel in-situ and green method with the combination of TiCl4 pretreatment and solvothermal growth was proposed to prepare the Pt-free Cu2ZnSnS4 (CZTS) counter electrodes (CEs) on FTO substrate. It was found that TiCl4 pretreatment toward the substrates was crucial to a high quality and high efficiency CZTS film, which consists of nanosheet and nanoparticle structure. The highly crystallized nanosheets were assembled from kesterite structure CZTS nanocrystals, with an average diameter of 10–30 nm. The detailed morphology, crystal structure, and composition of the CZTS nanostructures were characterized by SEM, TEM, SAED, XRD, Raman, and EDS analysis, respectively. Electrocatalytic abilities of the films toward I–/I3– were verified through cyclic voltammograms (CV), electrochemical impedance spectroscopy (EIS), and Tafel polarization measurements. A maximum power conversion efficiency of 5.65% was achieved for a cell with CZTS 3, under 100 mW/cm2, which was higher than that of a cell with a commercial Pt counter electrode (4.96%). This high efficiency was mainly attributed to the good bonding strength between CZTS films and FTO substrate (RS = 4.41 Ω cm2), and higher electron-transfer process at the electrolyte/CE interface (high JSC), along with superior electrochemical catalytic ability (RCt = 2.40 Ω cm2). The in-situ prepared CZTS CEs are proven to be suitable for high efficiency Pt-free dye-sensitized solar cells (DSSCs), leading to significantly decrease of the cell cost and simplification of preparation process.
研究领域:
材料科学
·
能源科学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Advanced Energy Materials
·
2025
·
IF 26
Guimei Liu,Yushen Liu,Xiaoyi Qiu,Bingxing Zhang,Juhee Jang,Yingdan Cui,Fei Xiao,Qinglan Zhao,Wenjun Wang,Yoonseob KIM,Wei Xing,Minhua Shao
The slow reaction kinetics of hydrogen oxidation reaction (HOR) on existing catalysts in alkaline hinders the commercialization of anion exchange membrane fuel cells (AEMFCs). In this work, a Cu-incorporated NiW alloy (Cu i -NiW) without any platinum group metal (PGM) is designed and evaluated in both liquid cells and AEMFCs. This catalyst enabled the achievement of an electrochemical surface area-normalized exchange current density of 70 µA cm −2 and robust stability, outperforming most PGM-free catalysts. Furthermore, the incorporation of Cu into other systems such as NiMo and NiV using the same method also showcased excellent HOR activity and durability. The fuel cells assembled with Cu i -NiW as the anode and Pt/C or Fe-N-C as the cathode delivered peak power densities of 480 and 340 mW cm −2 , respectively. Experimental and theoretical studies reveal that the incorporated Cu is chemically inert but enhances the overall oxidation resistance of the catalysts. Moreover, it weakens hydrogen adsorption and promotes the adsorption of hydroxide ions, thereby enhancing the HOR activity significantly. These results may open a door for rational design of high-performance and durable PGM-free HOR catalysts.
研究领域:
电化学
·
催化材料
·
能源科学
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2022
·Vol. 169
·期 10
·106507
·
IF 4.386
Mengxue Huang,Ruimin Ding,Jie Yang,Wenwen Shi,Shufang Shi,Lifang Chen,Shanshan Liu,Xi Yin
Platinum group metal-free catalysts based on transition metal and nitrogen co-doped carbon materials are gaining attention for their applications in electrocatalysis. Nitrogen-coordinated metal sites (MNx) have been identified as the main active sites in PGM-free catalysts. Current synthetic approaches rely on the high-temperature treatment to introduce targeted electroactive MNx sites into the carbon matrix. In this study, we demonstrated the formation of MNx sites on Ni- and N-co-doped carbon templates via the solution-phase coordination with target metal ions, including Fe2+, Fe3+, and/ Co2+. The formation of MNx sites was confirmed via a combined approach of various physical characterization techniques, elemental analysis, and electrochemical analysis. The results indicate that the metal-vacancy-Nx sites in the template can coordinate with target ions to form electrochemically active MNx sites. By varying heat-treatment temperature, the amount of FeNx sites formed via coordination with Fe2+ ion can be tuned and correlated with the change of activity toward oxygen reduction reaction. The amount of MNx sites formed via solution-phase coordination with various ions followed the sequence of Co2+ > Fe2+ > Fe3+. These findings may further guide the future development of MNx-C electrocatalysts through this solution-phase coordination approach.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2016
·
IF 8.328
Yongqi Hua,Tingting Jiang,Kun Wang,Mingmei Wu,Shuqin Song,Yi Wang,Panagiotis Tsiakaras
Despite that nitrogen (N) and sulfur (S) co-doped ordered mesoporous carbon (OMC) as Pt-free catalyst for oxygen reduction reaction (ORR) shows a desirable performance, the synthesis method is always complicated and expensive, which greatly hinders its development and application. In the present work, a highly ordered mesoporous N and S co-doped carbon material is developed. The material is obtained by combining hard template and high-temperature pyrolysis method using cheap saccharin as a single-source molecular precursor, SBA-15 as the hard template and FeCl 3 as the catalyst to promote the carbonization process. It is found that the as-prepared SN-OMC catalyst, compared with the commonly used commercial Pt/C (20 wt.%), exhibits comparable ORR electrocatalytic activity with mainly four-electron (4e − ) process, superior stability and inertness to methanol in alkaline media, which could mainly benefit from the highly ordered mesoporous structure and the synergistic effect caused by the dual N and S doping. These advantages render SN-OMC a promising ORR electrocatalyst and a cheap alternative to Pt/C for practical fuel cell applications .
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 46
·26323-26329
·
IF 12.732
Wangjin Ji,Changhong Zhan,Deyu Li,Yong Xu,Ying Zhang,Lu Wang,Liangbin Liu,Yu Wang,Wenxing Chen,Hongbo Geng,Xiaoqing Huang
The hydrogen oxidation reaction (HOR) has recently attracted great attention, yet the poor performance of HOR over the platinum group metal-free (PGMs-free) catalysts in alkaline conditions strongly impedes the development of hydroxide-exchange membrane fuel cells. Here, we demonstrate that the phase and interface engineering of nickel carbide (Ni3C) nanobranches can significantly enhance the alkaline HOR performance. Specifically, such interface engineering is realized through a facile annealing treatment of a branched Ni3C nanostructure. As a promising PGMs-free HOR catalyst, the strong interfacial synergy of Ni/Ni3C significantly enhances the HOR performance in alkaline media, with the HOR activity being comparable to that of a commercial Pt/C catalyst, and it demonstrates excellent CO tolerance. Mechanism studies show that the interfacial synergy facilitates electron transfer from Ni to Ni3C and thus regulates the absorption strengths of *H and *OH. This work opens up a new avenue for the design of high-performance PGM-free catalysts for electrocatalysis and beyond.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF RARE EARTHS
·
2018
·
IF 2.524
Kezhong Wu,Jiajing Zhao,Yuanyuan Xiong,Bei Ruan,Mingxing Wu
Pt-free counter electrode (CE) composed of La 2 MoO 6 (La 2 O 3 -MoO 3 ) was successfully synthesized by simple pyrolysis of lanthanum acetate (C 6 H 9 O 6 La· x H 2 O) and hexaammonium heptamolybdate tetrahydrate ((NH 4 ) 6 Mo 7 O 24 ·4H 2 O). Furthermore, three proportions composites catalysts of La 2 MoO 6 @MWCNTs based on La 2 MoO 6 and multiwall carbon nanotubes (MWCNTs) were prepared and characterized as Pt-free catalyst for CE in dye-sensitized solar cells (DSSCs). The morphology and structure of La 2 MoO 6 @MWCNTs composites were determined by scanning electron microscopy, transmission electron microscope and X-ray diffraction. The electrochemical performance of La 2 MoO 6 @MWCNTs composite catalysts for CEs was determined by photocurrent-voltage measurements, cyclic voltammetry , electrochemical impedance spectroscopy , and Tafel polarization. The power conversion efficiencies of 4.68%, 4.87% and 5.06% are obtained for La 2 MoO 6 :MWCNTs with the mass ratios of 5:1, 3:1 and 1:1 towards the reduction of I 3 – to I – under the same conditions, respectively, which are superior to those of MWCNTs (3.94%) and La 2 MoO 6 (1.71%) electrodes. The experimental results reveal that the presence of MWCNTs results in an augmented active catalytic surface area and enhanced charge transfer from CE to the electrolyte.
研究领域:
材料科学
·
能源科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Wanli Liang,Zhichen Le,Pengyu Dong,Zixuan Dan,Jiaxuan Chen,Hao Zhang,Jian Chen,Fangyan Xie,Nan Wang,Yanshuo Jin,Hui Meng
The development of hydrogen energy is limited by the high cost of platinum group metals (PGM). There is an urgent need to design efficient PGM-free electrocatalysts in the hydrogen electrode. Herein, Janus Ni/W bimetallic materials are proposed as an effective PGM-free bifunctional hydrogen electrocatalyst. By constructing the bimetallic materials, a synergistic effect is realized to enhance the reaction kinetics and improve the catalytic performance. In general, Ni can provide excellent H ad sites, and W serves as OH ad sites. Therefore, the synergistic effect of Ni and W can improve the kinetics of hydrogen evolution reaction and the hydroxide oxidation reaction. Ni/W@NF can obtain the hydrogen evolution reaction current density of 10 mA cm −2 with an overpotential of only 62.6 mV, and the exchange current density of hydroxide oxidation reaction can reach 1.83 mA cm −2 . This work provides a new idea for the design of high-efficiency and low-cost PGM-free bifunctional hydrogen electrocatalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Scientific Reports
·
2018
·Vol. 8
·期 1
·1-13
·
IF 4.122
Zhang Xiaoyan,Xu You,Zhang Junjie,Dong Shuai,Shen Liming,Gupta Arunava,Bao Ningzhong
Two-dimensional (2D) semiconducting nanomaterials have generated much interest both because of fundamental scientific interest and technological applications arising from the unique properties in two dimensions. However, the colloidal synthesis of 2D quaternary chalcogenide nanomaterials remains a great challenge owing to the lack of intrinsic driving force for its anisotropic growth. 2D wurtzite Cu 2 ZnSnS 4 nanosheets (CZTS-NS) with high-energy (002) facets have been obtained for the first time via a simple one-pot thermal decomposition method. The CZTS-NS exhibits superior photoelectrochemical activity as compared to zero-dimensional CZTS nanospheres and comparable performance to Pt counter electrode for dye sensitized solar cells. The improved catalytic activity can be attributed to additional reactive catalytic sites and higher catalytic reactivity in high-energy (002) facets of 2D CZTS-NS. This is in accordance with the density functional theory (DFT) calculations, which indicates that the (002) facets of wurtzite CZTS-NS possess higher surface energy and exhibits remarkable reducibility for I 3
− ions. The developed synthetic method and findings will be helpful for the design and synthesis of 2D semiconducting nanomaterials, especially eco-friendly copper chalcogenide nanocrystals for energy harvesting and photoelectric applications.
研究领域:
材料科学
·
能源技术
·
纳米科技
·
光电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 14
·5544
·
IF 4.6
Min Wang,Shilin Zhang,Juejin Teng,Shunsheng Zhao,Zhongtao Li,Mingbo Wu
An efficient and low-cost oxygen catalyst for the oxygen reduction reaction (ORR) was developed by in situ growth of Mn-Mo oxide nanoparticles on nitrogen-doped carbon nanotubes (NCNTs). Doped nitrogen effectively increases the electron conductivity of the MnMoO4@NCNT complex and the binding energy between the Mn-Mo oxide nanoparticles and carbon nanotubes (CNTs), leading to fast charge transfer and more catalytically active sites. Combining Mn and Mo with NCNTs improves the catalytic activity and promotes both electron and mass transfers, greatly enhancing the catalytic ability for ORR. As a result, MnMoO4@NCNT exhibited a comparable half-wave potential to commercial Pt/C and superior durability, demonstrating great potential for application in renewable energy conversion systems.Keywords:MnMoO4/NCNT composites;nitrogen doping;oxygen reduction reaction;platinum group metal (PGM)-free catalyst;electrocatalysis
研究领域:
材料科学
·
能源科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2019
·
IF 3.131
Liansheng Ma,Jingxin Kang,Yong Liu,Haifeng He
Fe-Co nanoparticle-incorporated carbon nanofibers ((Fe-Co)-CNFs) were obtained by a simple and flexible electrospinning method and were further pre-oxidized and carbonized under a high-temperature nitrogen atmosphere for application as counter electrodes for highly efficient platinum-free dye-sensitized solar cells (DSSCs). Electrochemical characterizations revealed that the (Fe-Co)-CNFs showed excellent electrocatalytic activity for the I 3 − /I − redox couple. Photoelectric performance tests have shown that dye-sensitized solar cells equipped with (Fe-Co)-CNF counter electrodes have comparable photovoltaic efficiency to platinum counter electrode cells. This is because the graphite properties of these fibers rendered them electronically conducting. One-dimensional nanofibers provide oriented electron transport pathways, while lapped fibers form a three-dimensional mesoporous network, enhancing the contact with the electrolyte, and hence leading to faster ionic reaction kinetics. This study demonstrates that (Fe-Co)-CNFs can be used as low-cost high-efficiency counter electrodes for DSSCs.
研究领域:
材料科学
·
能源技术
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xing Qian,Chong Xu,Yiqing Jiang,Jie Zhang,Guoxiang Guan,Yixuan Huang
Multi-shelled micro-/nanomaterials with complex hollow structures have been regarded as a promising kind of advanced catalysts for energy conversion owing to their large specific surface, increased active sites, and shortened paths of charge transfer. Herein, a series of double-shelled transition metal chalcogenides (Ni-Co-MoS x , Co-MoS x , and Ni-MoS x ) with ball-in-ball hollow structures have been synthesized by converting corresponding metal-glycerol spherical precursor with the assistance of (NH 4 ) 2 MoS 4 under a facile solvothermal condition. In this process, (NH 4 ) 2 MoS 4 acted as a multifunctional vulcanizator, which could conveniently afford Mo and S elements at the same time, and the mass ratio of the precursor to (NH 4 ) 2 MoS 4 played an indispensable role in preparing the uniform hollow sphere with satisfactory morphology and catalytic performance. Noteworthily, compared with ternary Co-MoS x and Ni-MoS x , the quaternary Ni-Co-MoS x ball-in-ball nanospheres demonstrated much enhanced catalytic properties in accelerating the reduction of triiodide in dye-sensitized solar cells (DSSCs) and the electrochemical hydrogen evolution reactions (HERs) due to the advantages of multi-elements, moderated surface texture, and larger surface area. Specifically, a prominent power conversion efficiency of 9.63% was achieved by the DSSC assembled with Ni-Co-MoS x counter electrode (CE), which was much superior to that of Pt CE (8.28%). Besides, Ni-Co-MoS x showed a low η 10 of 93.4 mV and a small Tafel slope of 55.0 mV dec −1 when employed as electrocatalysts for HER in 0.5 M H 2 SO 4 .
研究领域:
材料科学
·
能量转换
·
催化
·
纳米技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）