Small
·
2024
·
IF 13
Wentao Qu,Jian Zhu,Guozhong Cao,Shulin Chen,Yongwen Tan,Baohui Chen,Ming Zhang
Zinc-iodine batteries (Zn-I2) are extremely attractive as the safe and cost-effective scalable energy storage system in the stationary applications. However, the inefficient redox kinetics and “shuttling effect” of iodine species result in unsatisfactory energy efficiency and short cycle life, hindering their commercialization. In this work, Ni single atoms highly dispersed on carbon fibers is designed and synthesized as iodine anchoring sites and dual catalysts for Zn-I2 batteries, and successfully inhibit the iodine species shuttling and boost dual reaction kinetics. Theoretical calculations indicate that the reinforced d-p orbital hybridization and charge interaction between Ni single-atoms and iodine species effectively enhance the confinement of iodine species. Ni single-atoms also accelerate the iodine conversion reactions with tailored bonding structure of I─I bonds and reduced energy barrier for the dual conversion of iodine species. Consequently, the high-rate performance (180 mAh g −1 at 3 A g −1 ), cycling stability (capacity retention of 74% after 5900 cycles) and high energy efficiency (90% at 3 A g −1 ) are achieved. The work provides an effective strategy for the development of iodine hosts with high catalytic activity for Zn-I2 batteries.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Qiaona Liu,Xin Han,An Qian,Xin Pu,Lei Ye,Pengpeng Liu,Fengqi Zhang,Jichang Liu
Developing noble-metal-free dual-metal single-atom catalysts with rich active accessible sites and excellent catalytic activity is very meaningful and challenging, especially for photocatalytic hydrogen production reaction, which can significantly reduce the cost of photocatalytic technology application while reducing the use of noble metals. Herein, a novel noble-metal-free dual CuNi single-atom modified ZnIn 2 S 4 (CuNi SA -ZIS) photocatalyst with high hydrogen production performance were successfully prepared by a hydrothermal method. The ZnIn 2 S 4 with a spherical nanoflower structure is composed of ultrathin nanosheets, and AC HDDAF-STEM results shows that CuNi bimetallic particles are uniformly distributed on the surface of ZnIn 2 S 4 nanosheets and exhibit atomic level dispersion, forming dual-metal single-atom structure. The optimized 1 wt% CuNi SA -ZIS photocatalyst with the Cu/Ni ratio of 1:1 shows the optimum H 2 evolution performance with a rate of up to 7844.7 μmol· g −1 · h −1 using triethanolamine as a sacrificial reagent, which is significantly improved compared to pristine ZIS, Cu-ZIS and Ni-ZIS samples under simulated sunlight. Electrochemical and spectroscopic characterization results demonstrated that the improved photocatalytic activity of CuNi SA -ZIS was mainly due to the addition of the dual CuNi single atoms with a synergistic effect served as a co-catalyst for ZnIn 2 S 4 photocatalysts, providing efficient active sites for hydrogen evolution while preventing the fast recombination of photo-generated electrons and holes. This study provides a valuable source of ideas for the design of effective noble-metal-free dual-metal single-atom catalysts.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
CARBON
·
2021
·
IF 9.594
Yuxiang Liu,Xuejun Xu,Sufan Zheng,Shangchun Lv,Hewen Li,Zhichun Si,Xiaodong Wu,Rui Ran,Duan Weng,Feiyu Kang
Aluminum-doped strontium titanate SrTiO 3 (Al), has been demonstrated as the suitable photocatalyst for overall water splitting. Noble metals, such as RhCrO x , are widely applied to accelerate the photocatalytic hydrogen evolution . Herein, Ni single atoms anchored on nitrogen-doped graphene (Ni SA-NG) are adopted to replace noble metal as hydrogen (H 2 ) evolution cocatalysts for SrTiO 3 (Al)/CoO x photocatalyst. The prepared Ni SA-NG/SrTiO 3 (Al)/CoO x photocatalyst exhibits remarkable activity for photocatalytic overall water splitting with the H 2 evolution rate of 498 μmol g −1 h −1 and oxygen (O 2 ) evolution rate of 230 μmol g −1 h −1 , respectively. Ni SA-NG not only improves the efficiency of photogenerated charge transfer and separation through the Ti–O–C bonds acting as the electron transfer freeway, but also provides highly active sites to accelerate the surface H 2 evolution rate. This research provides a valuable method to construct SrTiO 3 -based photocatalyst without noble metal cocatalysts.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
DOI
高影响因子
MICROCHIMICA ACTA
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2024
·Vol. 191
·期 6
·1-15
·
IF 5.3
Yin Hang,Bai Xiao,Zhang Fanjun,Yang Ziyin
Single atom catalysts (SACs) have attracted attention due to their excellent catalysis activity under specific reactions and conditions. However, the low density of SACs greatly limits catalytic performance. The three-dimensional graphene hollow nanospheres (GHSs) with very thin shell structure can be used as excellent carrier materials. Not only can its outer surface be used to anchor metal single atoms, but its inner surface can also provide rich sites. Here, a novel step-by-step assembly strategy is reported to anchor nickel single atoms (Ni SAs) on the inner and outer surfaces of GHSs (Ni SAs/GHSs/Ni SAs), which significantly increases the loading capacity of Ni SAs (4.8 wt%). Compared to conventional materials that only anchor Ni SAs to the outer surface of the carrier (Ni SAs/GHSs), Ni SAs/GHSs/Ni SAs exhibits significantly higher electrocatalytic activity toward glucose oxidation in alkaline media. The sensitivity of Ni SAs/GHSs/Ni SAs/GCE is nearly five times higher than that of Ni SAs/GHSs/GCE. Moreover, the sensor based on Ni SAs/GHSs/Ni SAs can detect glucose in a wide concentration range of 0.8 µM–1.1244 mM with a low detection limit of 0.19 µM (S/N = 3). This study not only provides an effective sensing material for glucose detection, but also opens a new avenue to construct high-density metal SACs. Graphical Abstract
研究领域:
材料科学
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生物医学工程
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2024
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IF 14
Mingdong Sun,Wenwen Guan,Cailing Chen,Chao Wu,Xiaoling Liu,Biao Meng,Tao Chen,Yu Han,Jun Wang,Shibo Xi,Yu Zhou
The synergy of single atoms (SAs) and nanoparticles (NPs) has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction (CO 2 RR); however, the rationalization of the SAs/NPs proportion remains one challenge for the catalyst design. Herein, a Ni 2+ -loaded porous poly(ionic liquids) (PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer, 1-allyl-3-vinylimidazolium chloride, was pyrolyzed to prepare the Ni, N co-doped carbon materials, in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing temperature. The catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO 2 into CO. Operando Ni K -edge X-ray absorption near-edge structure (XANES) spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and NPs. The charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active sites. In the electroreduction of CO 2 , the co-existence of Ni SAs and NPs strengthened the CO 2 activation and the affinity towards the key intermediate of *COOH, lowering the free energy for the potential-determining *CO 2 → *COOH step, and therefore promoted the catalysis efficiency.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Yao Rui,Sun Kaian,Zhang Kaiyang,Wu Yun,Du Yujie,Zhao Qiang,Liu Guang,Chen Chen,Sun Yuhan,Li Jinping
Continuous and effective hydrogen evolution under high current densities remains a challenge for water electrolysis owing to the rapid performance degradation under continuous large-current operation. In this study, theoretical calculations, operando Raman spectroscopy, and CO stripping experiments confirm that Ru nanocrystals have a high resistance against deactivation because of the synergistic adsorption of OH intermediates (OH ad ) on the Ru and single atoms. Based on this conceptual model, we design the Ni single atoms modifying ultra-small Ru nanoparticle with defect carbon bridging structure (UP-RuNi SAs /C) via a unique unipolar pulse electrodeposition (UPED) strategy. As a result, the UP-RuNi SAs /C is found capable of running steadily for 100 h at 3 A cm −2 , and shows a low overpotential of 9 mV at a current density of 10 mA cm −2 under alkaline conditions. Moreover, the UP-RuNi SAs /C allows an anion exchange membrane (AEM) electrolyzer to operate stably at 1.95 V cell for 250 h at 1 A cm −2 .
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yibo Guo,Sai Yao,Yuanyuan Xue,Xu Hu,Huijuan Cui,Zhen Zhou
The electrochemical reduction reaction of carbon dioxide (CO 2 RR) is an effective way towards carbon neutralization. Single-atom catalysts (SACs) are expected to be efficient for CO 2 RR due to maximum atom utilization and excellent catalytic performance. Here, nitrogen-doped carbon supported Ni SACs (Ni-SAC@NCs) were prepared through effective fast pyrolysis . CO 2 can convert into CO efficiently with Ni-SAC@NCs as electrocatalysts for CO 2 RR. The faradaic efficiency kept well above 80% in the applied potential window of −0.6 to −0.9 V (vs. reversible hydrogen electrode (RHE)), with a highest FE CO of 95% at −0.6 V (vs. RHE). Ni-SAC@NCs can achieve the best CO selectivity under a small overpotential, surpassing most other state-of-the-art catalysts. Computations also indicate that the unique defect-Ni-N 3 structure is the active site. This work not only provides a simple and promising new route for the preparation of SACs, but also proves the key role of the coordination environment in electrocatalysis.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Shujin Shen,Cheng Han,Bing Wang,Yiang Du,Yingde Wang
Electroreduction of aqueous CO 2 is a sustainable approach to produce tunable syngas, which demands the rational design of dual-active-sites catalysts for individual CO 2 reduction reaction (CRR) and hydrogen evolution reaction (HER). Here, the self-supporting nickel@nitrogen-doped carbon nanotubes grown on carbon nanofiber (Ni@NCNTs-CNF) is developed with Ni single atoms (SAs) and nanoparticles (NPs) functioning as CRR and HER sites respectively. Benefiting from the hierarchical nanostructures for effective electron transport and mass diffusion, as well as the high accessibility of dual-active sites, Ni@NCNTs-CNF catalysts can mediate aqueous CO 2 into CO/H 2 (2:1) with a 100 % Faraday efficiency and a high current density (25 mA cm −2 ) at low working potential (-0.8 V). By manipulating the Ni SAs/Ni NPs ratio, the CO/H 2 proportion is easily modulated in a wide range from 1:4 to 5:1, independence of the working potential (-0.6 to -0.8 V). Our findings provide fresh insights into the design of dual-active-sites catalysts.
研究领域:
材料科学
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电化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Kui Wang,Bin Chen,Yimin Xuan,Wenjun Fan,Nan Sun,Sheng Chang,Guowen Meng
The CO 2 electroreduction (CO 2 RR) is extensively deemed as a promising route to reach carbon neutralization, while the single-atom catalysts (SACs) are proved to be effective in CO 2 RR. However, most SACs cannot further amplify performance due to their powdery feature. Herein, we present numerous isolated nickel single atoms anchored on 3D interconnected N-doped carbon tubes (NiSAs@3D-INCT) network as a self-supported electrode. The NiSAs@ 3D-INCT has truly interconnected and highly ordered vertical and lateral carbon tube-channels, which promote the CO 2 interaction and electrolyte transmission. The NiSAs@3D-INCT exhibits a superior CO 2 RR performance with an appreciable CO partial current density of 51.8 mA cm −2 at − 0.96 V versus the reversible hydrogen electrode (RHE). X-ray absorption fine structure spectroscopy and theoretical computations reveal the NiSAs are loaded on the 3D-INCT network with Ni-N 4 configuration as highly active sites for CO 2 RR. This work will shed a new light on opening up high performance SACs for CO 2 RR.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Xiao Bai,Hang Yin,Ziyin Yang
The content of metal single atoms is an important factor for restricting the electrocatalytic activity. In this work, the substitution-encapsulation strategy was reported to obtain high-density nickel single atoms (Ni SAs). This strategy was not only based on ion exchange between Zn nodes and adsorbed Ni2+ ions but also utilized porous ZIF-8 as a host to trap metal precursor guests in situ in their cages. The synergistic effect of ion exchange and precursor encapsulation significantly increased the content of Ni SAs. The structures of the Ni SAs were studied via transmission electron microscopy (TEM), high-angle annular dark-field scanning TEM (HAADF-STEM), X-ray diffractometry (XRD), X-ray photoelectron spectroscopy (XPS), and atomic absorption spectroscopy (AAS). Electrochemical studies revealed that the prepared high-density Ni SA catalyst is beneficial for increasing the electrocatalytic activity toward glucose. The sensitivity and the detection limit were 653.9 μA·mM–1·cm–2 and 0.51 μM, respectively. Furthermore, a sensor based on high-density Ni SAs can achieve highly sensitive determination of glucose content in energy drinks and serum samples. This work provides an idea for designing highly active electrocatalysts to improve glucose electrochemical sensing.
研究领域:
材料科学
·
电化学
·
生物传感器
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产品关联
DOI
高影响因子
Nano Research
·
2023
·Vol. 16
·期 7
·8800-8808
·
IF 9.9
Yang Shengshu,Zhang Fang,Qiu Haifa,Yang Ming,Qin Fengjuan,Tang Hao,Chen Wenxing,Liu Zhengang
Exploiting inexpensive and effective nickel-based catalysts that produce hydrogen from liquid organic hydrogen carriers (LOHCs) is crucial to alleviating the global energy and environmental crisis. In this study, we report a rational strategy that can realize atomically dispersed Ni atoms anchored on vacancy-abundant boron nitride nanosheets (Ni 1 / h -BNNS) with high specific surface area (up to 622 m 2 ·g −1 ) and abundant hydroxyl groups for high efficient hydrogen production. Methanol dehydrogenation results show an excellent hydrogen production performance catalyzed by this Ni 1 / h -BNNS, as evidenced by a remarkably high H 2 yield rate (1684.23 \({\rm{mol}} \cdot {\rm{mo}}{{\rm{l}}_{{\rm{Ni}}}}^{-1} \cdot {{\rm{h}}^{-1}}\) ), nearly 100% selectivity toward hydrogen and CO, and high anti-coking performance. Density functional theory (DFT) calculations reveal that the outstanding catalytic performance of Ni 1 / h -BNNS primarily originates from the unique coordinated environment of atomically dispersed Ni (Ni-B 2 O 2 ) and the synergistic interaction between Ni single atoms and the h -BNNS support. Specifically, the coordinated O atoms play a decisive role in promoting the activity of Ni, and the neighboring B sites significantly decrease the energy barriers for the adsorption of key intermediates of methanol dehydrogenation. This study offers a novel strategy for developing high-performance and stable single-atom Ni catalysts by precisely controlling single-atom sites on h -BN support for sustainable hydrogen production.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Min Li,Ye Hu,Wenhui Fang,Shixian Xin,Ying Wu,Yutao Cao,Wei Cui,Zengxi Li,Hong Zhao
The intrinsic performance of single atom catalysts (SACs) to electrochemical CO 2 reduction reaction (ECRR) is limited due to the absence of synergistic active sites. Herein, Ni single atom (Ni SAs ) and Ni nanoparticles (Ni NPs ) are co-loaded on nitrogen-doped hollow carbon spheres (N-HCSs) by a one-step calcination method, which exhibits high CO selectivity in H-type cell with aqueous solution or an ionic liquid as electrolyte. Particularly, Ni SAs-NPs -N-HCSs demonstrate a CO selectivity of 98.98%, yielding an industrial level CO current density of 152.7 mA cm −2 in flow cell. In situ Raman spectroscopy and in situ infrared characterization technology confirm that *COOH and *CO are important intermediates in the ECRR process. Theoretical computations suggest that coexisting Ni NPs can reduce the energy barrier of *COOH, thereby improving the ECRR performance, indicating the synergistic effect between Ni SAs and Ni NPs in the ECRR process. Moreover, Ni SAs-NPs -N-HCSs is applied to the membrane electrode assembly system coupling the hydrazine oxidation reaction (HzOR), which can significantly reduce the voltage about 836 mV at 100 mA cm −2 .
研究领域:
材料科学
·
电化学
·
催化反应
✓ 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）