ACS Nano
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2025
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IF 16
Yaxi Gan,Ataollah Kalantari Osgouei,Alexander Ahrens,Bofang Wang,Jingyi Zhou,Jun-Zheng Zhan,Dan Zeng,Shengqiang Nie,Xinyuan Zhao,Guangxu Chen,Peter Nordlander,Linan Zhou
Plasmonic photocatalysis is promising for solar-driven chemical transformations under mild conditions; however, conventional materials like aluminum, copper, silver, and gold are resonant at short wavelengths, limiting their use in the red to near-infrared sunlight spectrum. In this study, we have developed a class of antenna-reactor (AR) photocatalyst based on two-dimensional (2D) plasmonic materials, Ti3C2Tx, also known as MXenes. A Ru-loaded Ti3C2Tx plasmonic photocatalyst achieves a turnover frequency of approximately 2 s–1 and energy efficiency of 10% for hydrogen production under 660 nm light excitation, being 2–3 orders of magnitude superior to the performance achieved in thermocatalysis. This 2D plasmonic antenna demonstrates superiority over the benchmark CuRu surface-alloy AR structure in hot-electron-driven processes under red light excitation. Kinetic studies suggest that the rate-determining step in both photo- and thermocatalysis is nitrogen’s associative desorption. Hot electrons enhance activity by promoting the removal of adsorbed nitrogenous species.
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
Journal of Materials Chemistry C
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2024
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IF 5.7
Xiaoying Yu,Tianfang Zheng,Yuanlin Li,Yanxiang Liu,Ping Guo,Hai-Hua Wang,Shin-ichi Sasaki,Xiao-Feng Wang
The production of hydrogen fuel by solar-driven photocatalytic water splitting is an attractive solution to overcome the environmental and energy problems with traditional fossil fuels. The strategies to improve the capacity of photocatalytic hydrogen production include enhancing the light absorption of materials and using co-catalysts to reduce the efficiency of electron–hole recombination. Here, we report a Schottky heterojunction photocatalyst composed of subphthalocyanine (SubPc) and Ti3C2Tx MXene, which can effectively separate photogenerated charges. The outstanding ability of SubPc to absorb visible light and the ability of Ti3C2Tx MXene to capture photogenerated electrons were applied to improve the photocatalytic hydrogen-production performance of the SubPc/Ti3C2Tx composite. Two types of SubPcs (SubPc-Cl and SubPc-OPh) were hybridized with Ti3C2Tx MXene nanosheets. The hydrogen evolution of SubPc/Ti3C2Tx with different mass ratios was experimentally investigated, and it was found that the optimized SubPc-Cl/Ti3C2Tx exhibited the best H2-production rate of 105 μmol g−1 h−1. Our findings provide a new design approach and promising strategy to develop low-cost photocatalysts for future solar-driven sustainable energy-conversion systems.
研究领域:
材料科学
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能源转换
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光化学
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DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 30
·2401694
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IF 27.4
Yin Zhu,Yanxu Chen,Yafei Feng,Xiangmin Meng,Jing Xia,Genqiang Zhang
Hydrazine oxidation-assisted water splitting is a critical technology to tackle the high energy consumption in large-scale H 2 production. Ru-based electrocatalysts hold promise for synergetic hydrogen reduction (HER) and hydrazine oxidation (HzOR) catalysis but are hindered by excessive superficial adsorption of reactant intermediate. Herein, this work designs Ru cluster anchoring on NiFe-LDH (denoted as Ru c /NiFe-LDH), which effectively enhances the intermediate adsorption capacity of Ru by constructing Ru─O─Ni/Fe bridges. Notably, it achieves an industrial current density of 1 A cm −2 at an unprecedentedly low voltage of 0.43 V, saving 3.94 kWh m −3 H2 in energy, and exhibits remarkable stability over 120 h at a high current density of 5 A cm −2 . Advanced characterizations and theoretical calculation reveal that the presence of Ru─O─Ni/Fe bridges widens the d-band width (W d ) of the Ru cluster, leading to a lower d-band center and higher electron occupation on antibonding orbitals, thereby facilitating moderate adsorption energy and enhanced catalytic activity of Ru.
研究领域:
材料科学
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电化学
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能源技术
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PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 42
·22819-22833
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IF 14.511
Renzhi Xiong,Changcun Tang,Kunjiao Li,Jiabao Wan,Weifeng Jia,Yanhe Xiao,Baochang Cheng,Shuijin Lei
It is an effective method to promote the activity of photocatalysts by exploiting their own photothermal effects to increase the temperature of the reaction center and thus accelerate the kinetic process of photocatalysis. In this study, for the first time, a CoCr2O4/g-C3N4 composite photocatalyst is designed through the construction of CoCr2O4 nanoparticles decorated tremella-like porous g-C3N4. On the one hand, the type-II heterostructure can be formed and effectively improves the separation efficiency of photogenerated carriers. On the other hand, the photothermal effect of plasmonic CoCr2O4 nanoparticles can significantly increase the temperature of the reaction system, thereby enhancing the photocatalytic efficiency. CoCr2O4 nanoparticles exhibit a broad-band strong absorption in the near-infrared region. Under full spectrum illumination for 300 s, their surface temperature can be increased by 113 °C, demonstrating excellent photothermal properties. Although the bare CoCr2O4 nanoparticle sample does not show the photocatalytic activity of water splitting for hydrogen evolution, the optimized g-C3N4/CoCr2O4 heterostructure composite exhibits an average hydrogen production rate as high as 1525.1 μmol g−1 h−1 under UV-Vis-IR illumination, which is 4.0 and 5.8 times higher than that of bare g-C3N4 under UV-Vis-IR and UV-Vis light illumination, respectively. This work provides a new guide for designing novel photothermal-assisted photocatalytic composite materials.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Tingyuan Zhang,Lingxiao Song,Jiahui Yang,Jiajia Wang,Dong Feng,Baojun Ma
Heteroatom doping is a promising strategy for optimizing the photocatalytic activity of semiconductors. However, relying solely on single-element doping often poses challenges in modulating the capabilities of semiconductors. Herein, we adopt a strategy of simultaneously modifying ZnIn 2 S 4 with the double non-metallic elements nitrogen (N) and oxygen (O) to form (N, O)-ZnIn 2 S 4 . Interestingly, (N, O)-ZnIn 2 S 4 exhibits significantly higher hydrophilicity and specific surface area compared to pristine ZnIn 2 S 4 . The contact angle decreases from 24° to 21°, while the specific surface area increases from 56 m 2 /g to 75 m 2 /g. The hydrogen production rate of (N, O)-ZnIn 2 S 4 reaches 400 μmol/h/g, which is 2.52 times higher than that of pristine ZnIn 2 S 4 . Photoelectrochemical characterization reveals that (N, O)-ZnIn 2 S 4 has a lower overpotential, higher photocurrent, lower resistance, reduced fluorescence intensity, and shorter fluorescence lifetime. Additionally, co-catalyst loading boosts the hydrogen production activity of ZnCo 2 S 4 /(N, O)-ZnIn 2 S 4 from 548 μmol/h/g to 810 μmol/h/g, compared to ZnCo 2 S 4 /ZnIn 2 S 4 . This study presents a dual non-metallic modification strategy to enhance semiconductor properties, achieving superior performance in photocatalytic hydrogen production.
研究领域:
材料科学
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能源科学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Yu-Chuan Jiang,Hui-Ying Sun,Ya-Nan Li,Jia-Wei He,Qi Xue,Xinlong Tian,Fu-min Li,Shi-Bin Yin,Dong-Sheng Li,Yu Chen
Methanol electrolysis is a promising strategy to achieve energy-saving and efficient electrochemical hydrogen (H2) production. In this system, the advanced electrocatalysts with high catalytic performance for both the methanol oxidation reaction (MOR) and hydrogen evolution reaction (HER) are highly desirable. Inspired by the complementary catalytic properties of rhodium (Rh) and palladium (Pd) for MOR and HER, herein, several Pd core–RhPd alloy shell nanodendrites (Pd@RhPd NDs) are synthesized through the galvanic replacement reaction between Pd nanodendrites (Pd NDs) and rhodium trichloride. For MOR, Pd@RhPd NDs exhibit Rh content-determined catalytic activity, in which Pd@Rh0.07Pd NDs have an optimal combination of oxidation potential and oxidation current due to the synergistic catalytic process of Pd/Rh double active sites. For HER, the introduction of Rh greatly improves the catalytic activity of Pd@RhPd NDs compared to that of Pd NDs, suggesting that Rh is the main activity site for HER. Unlike MOR, however, the HER activity of Pd@RhPd NDs is not sensitive to the Rh content. Using Pd@Rh0.07Pd NDs as robust bifunctional electrocatalysts, the as-constructed two-electrode methanol electrolysis cell shows a much lower voltage (0.813 V) than that of water electrolysis (1.672 V) to achieve electrochemical H2 production at 10 mA cm–2, demonstrating the application prospect of methanol electrolysis for H2 production.
研究领域:
材料科学
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电化学
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能源科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lijuan Yang,Yujie Zhao,Lijun Zhu,Daohong Xia
Superionic conductors regulated transition metal chalcogenides are the newly emerged electrocatalyst in water electrolysis into clean hydrogen and oxygen. However, there is still much room for the development of structural design, electronic modulation and heterogeneous interface construction to improve the overall water splitting performance in pH-universal solutions, especially in alkaline and neutral mediums. Herein, using β-cyclodextrin (β-CD) and citric acid (CA) organics with abundant hydroxyl (–OH) and carboxyl (–COOH), a special Ag 2 Se nanoparticles-decorated CoSe 2 flower-like nanosheets loaded on porous and conductive nickel foam substrate (Ag 2 Se-CoSe 2 /NF) was successfully constructed by a new method of monometallic cation release of coordinated cobalt. The Ag 2 Se phase exerts the nature characteristics of superionic conductors to modulate the morphological and electronic structures of CoSe 2 as well as improve its conductivity. The generated rich active interfaces and abundant Se vacancy defects facilitate numerous active sites exposure to accelerate the hydrogen ion transport and charge transfer. Compared to the single-phase Ag 2 Se/NF-8 and CoSe 2 /NF, the prepared Ag 2 Se-CoSe 2 /NF-8 with a two-phase synergistic effect achieves an outstanding pH-universal electrocatalytic hydrogen production performance by water electrolysis, as evidenced by a lower overpotential (60 mV, 212 mV and 85 mV vs RHE at 10 mA cm −2 for pH = 0.36, 7.00 and 13.70, respectively). Only a voltage of 1.55 V at 10 mA cm −2 is required to implement the overall water splitting in an alkaline electrolyzer. This work provides significant guidance for the future designation and practical development of transition metal chalcogenides with superionic conductors applied in the electrocatalytic field.
研究领域:
材料科学
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电催化
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能源转换
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产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2022
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IF 7.336
Fan Liu,Yang Tang,Jiaming Zhao,Yu Bai,Jiucun Chen,Liangliang Tian,Syed Shoaib Ahmad Shah,Shu-juan Bao
The insufficient intrinsic activity and electrical conductivity of transition metal-based catalysts still inhibits their practical application. In this work, carbon-coated nano-Ni-armed Mo 2 N nanosheets (Ni@C-Mo 2 N) assembled on Ni Foam (NF) by using CDs-NH 2 as reaction inducing and welding reagent. In-depth experiments reveal that the functional groups of (CDs) play a decisive role in regulating the phase composition and hierarchical structure of the final hybrid material. As electrocatalysts for hydrogen evolution reaction (HER), the optimized hierarchical Ni@C-Mo 2 N/NF achieved a very low overpotential of 38 mV at 10 mA cm −2 and outstanding stability of over 60 h, which should from the synergistic interfacial effect among the Ni, Mo 2 N and graphitic carbon optimized the electronic structure of catalyst with enhanced active sites, and improved electrical conductivity. This work provides novel insights for constructing more hierarchical multicomponent materials with the help of variable functional groups of CDs for further electrochemical applications.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Pan Li,Xinbao Li,Ye Yuan,Yang Wang,Pengfei Shen,Xinbo Zhu,Yingying Zhu
Steam reforming of bio-oil for hydrogen production is a promising green technology. Acetic acid was used as the bio-oil model compound. Experimental and density functional theory calculations were carried out to study the performance of Co/Al 2 O 3 catalysts doped with boron (B) with a 1 wt.%–5 wt.% content. Catalyst characterization by BET, XRD , XPS , NH 3 -TPD, H 2 -TPR, TEM, and TG-DTG was performed. We found that the catalyst performance improved significantly by B doping. Under the reaction conditions of T = 500 °C, steam-to-carbon ratio (S/C) = 5, and liquid hourly space velocity (LHSV) = 4.3 h −1 , the catalyst with a B doping ratio of 1 wt.% had the highest hydrogen yield of 85% and a maximum acetic acid conversion rate of 95%. The corresponding hydrogen productivity was 0.8 mmol/min. The stability of this catalyst exceeded 29 h. Density functional theory calculations showed that the interactions between the reaction intermediates and the surface were strengthened with B addition.
研究领域:
化学工程
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材料科学
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催化反应
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产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Chenyu Wang,Xiaolong Ling,Chaoyue Wu,Chao He,Biao Gui,Weibo Sun
Phosphorus is a very important resource, and dewatered cyanobacteria contains a large amount of it. Basic additives, such as KOH, are often used to promote hydrogen production during supercritical water gasification (SCWG) of biomass, but their effects phosphorus transformation have rarely been investigated. In this study, SCWG of dewatered cyanobacteria with potassium salt and KOH was conducted in autoclave at 400 °C for 10 min, to investigate the effect of K + on the transformation of phosphorus under neutral and alkaline conditions. Results showed that K + increased the proportion of phosphorus in the solid phase from 88.4% to 90.8–98.3%. Furthermore, K + could promote the transformation of iron-combined phosphorus to calcium-combined phosphorus and occluded phosphate. Only when the reaction environment was alkaline, the proportion of phosphorus in the solid phase was significantly reduced to a minimum of 26.1%. When the amount of OH − was sufficient, can this part of phosphorus and organic phosphorus , which was decomposed and transformed by the promotion of OH − , be transferred to the liquid products. Results from this study laid a foundation simultaneously for hydrogen production and phosphorus recovery more environmentally and high-effectively.
研究领域:
环境科学
·
生物化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Shenyan Zhou,Lianqing Yu,Qianlong Yang,Chong Liu,Wenjing Xie,Kehui Xue,Zhe Li,Yaping Zhang,Haifeng Zhu
The production of hydrogen via the photolysis of water represents a sustainable and environmentally benign approach to energy generation, which has the potential to mitigate energy shortages and environmental degradation. Nonetheless, the efficiency of photocatalysts is significantly limited by the effectiveness of charge carrier separation. Reducing the diffusion distance of these carriers can enhance their overall performance of the photocatalyst. In this context, a composite photocatalyst comprising CuNi 2 S 4 and ZnCdS was synthesized through one-step hydrothermal process. This bulk-phase heterojunction increases the nano-contact areas while maintaining an interface distance that is smaller than the diffusion distance of the carriers. Consequently, the optimal hydrogen production rate achieved was 33.87 mmol/g h, which is an order of magnitude greater than that of pure ZnCdS at 3.35 mmol/g h. Furthermore, the quantum efficiency at 400 nm reached 16 %. The photocurrent of the ZCS-CNS-3 % sample was 57.1 μA/cm², 4.35-fold of pure ZnCdS at 13.1 μA/cm². The incorporation of CuNi 2 S 4 significantly reduces the overpotential required for hydrogen evolution, while concurrently reducing the carrier transfer resistance by an order of magnitude. This bulk-phase structure not only broadens the prospects for the advancement of green and clean energy solutions but also enhances the methodologies for synthesizing nano-contact photocatalysts.
研究领域:
材料科学
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能源研究
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环境科学
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DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2024
·
IF 5.6
Chenlong Liu,Yijun Zhang,Yiman Xiao,Ruyue Zhang,Siddig Abuelgasim,Chenghua Xu,Atif Abdalazeez
Bio-oil by-products are inevitable with biomass gasification. It is considered a potential resource for hydrogen production via steam reforming. This study investigated acetic acid as a bio-model compound using a NiAl 2 O 4 catalyst. The effect of reaction conditions on hydrogen-rich production has also been discussed, including reaction time (1 h, 3 h, 5 h and 7 h), steam/carbon ratio (S/C = 1–4) and the blend of NiAl 2 O 4 and CaO (1:0, 3:1, 1:1, 1:3 and 0:1). The fresh and spent samples were characterized by XRD, XPS, SEM, BET, etc. The result showed that the CaO addition has several advantages: 1) it increases hydrogen gas purification; 2) it prevents Ni separation from NiAl 2 O 4 ; 3) it decreases the sintering of NiAl 2 O 4 . However, Ca 5 Al 6 O 14 formation decreases the activity of hydrogen production. In reaction conditions, steam is an essential factor for hydrogen gas production. The S/C ratio = 3 shows the optimum result for hydrogen gas production. Although the higher S/C ratio = 4 can maintain the adsorption activity of CaO, it causes Ni separation from NiAl 2 O 4 . The blend of NiAl 2 O 4 and CaO is another essential factor for hydrogen gas production. Adding CaO has increased hydrogen gas production significantly. However, a little CaO in a blend ratio 3:1 does not maintain the stability of the NiAl 2 O 4 structure. In the end, the optimum conditions are S/C ratio = 3 and blend = 1:1 at 650 °C, which produces hydrogen gas yield (2.1 mol/mol) and H 2 /CO (5.83).
研究领域:
能源科学
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催化化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）