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ELECTROCHIMICA ACTA · 2021 · IF 6.901

Ultrathin Ti2NTx MXene-wrapped MOF-derived CoP frameworks towards hydrogen evolution and water oxidation

Hui Zong,Ruijuan Qi,Ke Yu,Ziqiang Zhu

Hydrogen evolution is of great significance for reducing carbon emissions and realizing carbon-neutral. Hydrogen evolution reaction (HER) by water splitting has no carbon emissions and pollution, but it is still necessary to reduce cost and enhance catalytic activity. Herein, we report an ultra-thin Ti 2 NT x MXene-wrapped metal-organic frameworks (MOFs)-derived CoP composite (Ti 2 NT x @MOF-CoP), which is a bifunctional catalyst with low cost and high activity. We synthesize the Ti 2 NT x @MOF-CoP composite by phosphating the precursor ZIF-67 self-assembled with Ti 2 NT x MXene nanosheets. The Ti 2 NT x @MOF-CoP electrode shows competitive hydrogen evolution performance in a wide pH-range (current density of 10 mA cm −2 ) and has a low overpotential ( η ) of 112 mV in pH = 14 especially. The Ti 2 NT x @MOF-CoP electrode for OER also has a low η  = 241 mV at 50 mA cm −2 . Based on the bifunctional activity of Ti 2 NT x @MOF-CoP in alkaline, we set a dual-electrode configuration for HER and OER. It has a bias of 1.61 V at 10 mA cm −2 , with impressive catalytic stability during a 20 h measurement. MOFs-derived CoP has a large specific surface area and strong catalytic activity. Ti 2 NT x as a novel member of the MXene family not only can increase the active sites, but also can improve the stability of heterojunction catalysts. It reveals that the Ti 2 NT x @MOF-CoP composite has great potential in hydrogen evolution and water oxidation, thus reducing carbon emissions and protecting the environment.

研究领域: 材料科学 · 能源化学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-11 · IF 14.7

Oxophilic Ce single atoms-triggered active sites reverse for superior alkaline hydrogen evolution

Shen Fengyi,Zhang Zhihao,Wang Zhe,Ren Hao,Liang Xinhu,Cai Zengjian,Yang Shitu,Sun Guodong,Cao Yanan,Yang Xiaoxin,Hu Mingzhen,Hao Zhengping,Zhou Kebin

The state-of-the-art alkaline hydrogen evolution catalyst of united ruthenium single atoms and small ruthenium nanoparticles has sparked considerable research interest. However, it remains a serious problem that hydrogen evolution primarily proceeds on the less active ruthenium single atoms instead of the more efficient small ruthenium nanoparticles in the catalyst, hence largely falling short of its full activity potential. Here, we report that by combining highly oxophilic cerium single atoms and fully-exposed ruthenium nanoclusters on a nitrogen functionalized carbon support, the alkaline hydrogen evolution centers are facilely reversed to the more active ruthenium nanoclusters driven by the strong oxophilicity of cerium, which significantly improves the hydrogen evolution activity of the catalyst with its mass activity up to −10.1 A mg −1 at −0.05 V. This finding is expected to shed new light on developing more efficient alkaline hydrogen evolution catalyst by rational regulation of the active centers for hydrogen evolution.

CAS / MDL: 57-13-6
研究领域: 催化 · 材料科学 · 能源材料
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Nanomaterials · 2022 ·Vol. 12 ·期 9 ·1535 · IF 5.719

Electrospun Donor/Acceptor Nanofibers for Efficient Photocatalytic Hydrogen Evolution

Xiaoyu Lin,Yuanying Liang,Zhicheng Hu,Xi Zhang,Youcai Liang,Zhengwei Hu,Fei Huang,Yong Cao

We prepared a series of one-dimensional conjugated-material-based nanofibers with different morphologies and donor/acceptor (D/A) compositions by electrospinning for efficient photocatalytic hydrogen evolution. It was found that homogeneous D/A heterojunction nanofibers can be obtained by electrospinning, and the donor/acceptor ratio can be easily controlled. Compared with the single-component-based nanofibers, the D/A-based nanofibers showed a 34-fold increase in photocatalytic efficiency, attributed to the enhanced exciton dissociation in the nanofibrillar body. In addition, the photocatalytic activity of these nanofibers can be easily optimized by modulating the diameter. The results show that the diameter of the nanofibers can be conveniently controlled by the electrospinning feed rate, and the photocatalytic effect increases with decreasing fiber diameter. Consequently, the nanofibers with the smallest diameter exhibit the most efficient photocatalytic hydrogen evolution, with the highest release rate of 24.38 mmol/(gh). This work provides preliminary evidence of the advantages of the electrospinning strategy in the construction of D/A nanofibers with controlled morphology and donor/acceptor composition, enabling efficient hydrogen evolution.Keywords:photocatalysts;polymer blends;hydrogen evolution

研究领域: 材料科学 · 化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Construction 0D/2D heterojunction by highly dispersed Ag2S quantum dots (QDs) loaded on the g-C3N4 nanosheets for photocatalytic hydrogen evolution

Ziyi You,Xiaoyang Yue,Dainan Zhang,Jiajie Fan,Quanjun Xiang

In recent years, the use of quantum dots (QDs) cocatalysts to improve the hydrogen evolution activity from the water splitting of photocatalysts has become a popular research topic. Herein, we successfully prepared a novel 0 dimension/2 dimension (0D/2D) heterojunction nanocomposite (denoted Ag 2 S quantum dots (QDs)/g-C 3 N 4 ) with excellent photocatalytic performance by anchoring the Ag 2 S QDs cocatalyst on the surface of g-C 3 N 4 through a self-assembly strategy. Ag 2 S QDs with an average particle size of approximately 5.8 nm were uniformly and tightly modified on g-C 3 N 4 . The Ag 2 S QDs/g-C 3 N 4 composite with 0.5 wt% Ag 2 S QDs loading achieved the highest hydrogen evolution rate of 471.1 μmol·g −1 ·h −1 with an apparent quantum efficiency (AQE) of 1.48% at 405 nm. Such remarkable hydrogen evolution activity far exceeded that of undoped g-C 3 N 4 and Ag 2 S nanoparticles (NPs)/g-C 3 N 4 . Moreover, it was 2.04 times the activity of Pt/g-C 3 N 4 with Pt as the cocatalyst. The enhanced photocatalytic performance was attributed to the energy band broadening of Ag 2 S QDs caused by the quantum size effect and the convenient and effective charge transfer between g-C 3 N 4 and Ag 2 S QDs cocatalysts. The mechanism underlying the enhanced photocatalytic H 2 evolution activity was further proposed. This study demonstrates that semiconductor-based quantum dots are strong candidates for excellent cocatalysts in photocatalysis.

CAS / MDL: 108-78-1
研究领域: 材料科学 · 能源科学
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CERAMICS INTERNATIONAL · 2022 · IF 5.532

Lewis acid molten salts prepared Ti3C2Cl2 MXenes assembling with g-C3N4 nanosheets for enhanced photocatalytic H2 evolution

Hongmiao Zhou,Jiayi Tian,Ruoyu Wang,Difu Zhan,Peng Liu,Ruolin Chen,Yizhong Huang,Zhifeng Liu,Changcun Han

Photocatalytic hydrogen (H 2 ) evolution is expected to be a promising approach to generating a clean energy source (H 2 ) with low carbon emissions, which is vital to solving environmental degradation and energy shortages. The critical challenge to designing highly efficient photocatalysts is the fast recombination of photo-generated carriers; thus, we select Ti 3 C 2 Cl 2 MXene with excellent metal characteristics to serve as a co-catalyst and combine with g-C 3 N 4 . The Ti 3 C 2 Cl 2 /g-C 3 N 4 composites exhibit an enhanced photocatalytic hydrogen evolution activity (maximum 155.9 μmol h −1 ) while they hardly perform photocatalytic activities. The photoluminescence (PL) spectra shows that Ti 3 C 2 Cl 2 MXenes help boost the separation of photo-generated carriers of g-C 3 N 4 and finally strengthen the photocatalytic hydrogen evolution performance. The ultraviolet–visible (UV–vis) spectra illustrate that composites perform a strengthened light absorption, which fits well with the results in the hydrogen evolution experiment. Thus, we fabricated a highly efficient photocatalyst through a safer molten salt approach without hydrofluoric acid (HF). We believe this work will offer a safer approach to manufacturing catalysts decorated with MXenes for highly efficient photocatalytic H 2 evolution.

CAS / MDL: 12125-02-9 7646-85-7
研究领域: 材料科学 · 化学工程 · 能源科学 · 环境科学
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Materials Science and Engineering B-Advanced Functional Solid-State Materials · 2022 · IF 3.407

High efficient and stable Z-scheme g-C3N4/Zn0.5Cd0.5S photocatalyst driven by visible light for hydrogen evolution

Lianqing Yu,Xingyu Zhao,Jiandong He,Lijie Duan,Yankun Wang,Yaping Zhang,Haifeng Zhu

It is extremely desirable to develop efficient and cheap water splitting photocatalysts. An ultrahigh performance and stable photocatalyst g-C 3 N 4 /Zn 0.5 Cd 0.5 S was prepared by simple sintering method. g-C 3 N 4   nanosheets are evenly distributed around 20–30 nm ZnCdS nanoparticles, which can accelerate carriers separation and transfer, and increase the carriers life-time from 4.1 ns to 5.5 ns. UV–vis absorption spectra demonstrate that their absorption range can reach to visible light edge of 539 nm. The photocatalyst has a high photocatalytic hydrogen evolution rate of 16.66 mmol•h −1 •g −1 under visible light illumination (λ = 400–780 nm). Furthermore, after six recycles of photocatalyst, the hydrogen evolution stability still remains 94%. The excellent photocatalytic performance is attributed to the Z-scheme energy band structure formed between g-C 3 N 4 and Zn 0.5 Cd 0.5 S by simple sintering method. This work provides significant progress toward the synthesis of cheap Z-scheme photocatalysts for practical applications.

研究领域: 材料科学 · 能源化学
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ACS Applied Nano Materials · 2022 · IF 6.14

Quasi-Monolayer Ag2Se/1T-WSe2 Nanosheets for Enhanced Electrocatalytic Hydrogen Evolution and Charge Storage

Mairman Muska,Ye Wang,Jing Yang,Lin Ma,Qian Xu,Honghe Ding,Junfa Zhu,Qing Yang

With a dual strategy of phase-interface engineering, monolayer (1L)–1T-WSe2 integrated with Ag2Se nanoparticles (NPs) is in situ fabricated as quasi-monolayer Ag2Se/1L–1T-WSe2 hybrid nanosheets via a one-pot oleylamine-colloidal reaction. The Ag2Se NPs direct the growth of 1L–1T-WSe2 nanosheets forming the quasi-monolayer hybrid nanosheets by lodging in the interlayer spaces of WSe2 while the Ag2Se NPs being in a superionic conductor state diffuse rapidly and prevent the growth of piled-up multilayered WSe2 nanosheets. Due to the formation of quasi-monolayer Ag2Se/1L–1T-WSe2 nanosheets, many more side edges are exposed. Intensive studies illustrated that the quasi-monolayer Ag2Se/1L–1T-WSe2 hybrid nanosheets provide increased surface area and active sites as compared with isolated Ag2Se and WSe2. The hybrid nanosheets demonstrated excellent catalytic properties for hydrogen evolution reaction (HER) with overpotentials (η10) of 163 and 140 mV in acidic and basic conditions, respectively, and an outstanding alkaline supercapacitance of 1674 F g–1 at 1 A g–1. Meanwhile, X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS) determinations revealed that the quasi-monolayer hybrid nanosheets with enhanced electronic modulation could promote H+ adsorption/H2 desorption and accelerate the transport and separation of charge on the interface of heterostructured catalyst along with the electrode surface so as to exhibit outstanding electrochemical performances for HER and pseudocapacitance.

研究领域: 材料科学 · 电化学
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Nanomaterials · 2018 ·Vol. 8 ·期 10 ·835 · IF 3.504

Fabrication of ZnO/Red Phosphorus Heterostructure for Effective Photocatalytic H2 Evolution from Water Splitting

Jiaqi Chen,Shaolong Huang,Yaojia Long,Jiahao Wu,Hui Li,Zhao Li,Yu-Jia Zeng,Shuangchen Ruan

Photocatalysis is a green technique that can convert solar energy to chemical energy, especially in H2production from water splitting. In this study, ZnO and red phosphorus (ZnO/RP) heterostructures were fabricated through a facile calcination method for the first time, which showed the considerable photocatalytic activity of H2evolution. The photocatalytic activities of heterostructures with different ratios of RP have been investigated in detail. Compared to bare ZnO, ZnO/RP heterostructures exhibit a 20.8-fold enhancement for H2production and furthermore overcome the photocorrosion issue of ZnO. The improved photocatalytic activities highly depend on the synergistic effect of the high migration efficiency of photo-induced electron–hole pairs with the inhibited charge carrier recombination on the surface. The presented strategy can also be applied to other semiconductors for various optoelectronics applications.Keywords:photocatalysis;H2evolution;red P;ZnO;heterostructure

研究领域: 材料科学 · 能源科学
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Nanomaterials · 2019 ·Vol. 10 ·期 1 ·1 · IF 4.034

In Situ Construction of Ag/TiO2/g-C3N4 Heterojunction Nanocomposite Based on Hierarchical Co-Assembly with Sustainable Hydrogen Evolution

Rui Geng,Juanjuan Yin,Jingxin Zhou,Tifeng Jiao,Yao Feng,Lexin Zhang,Yan Chen,Zhenhua Bai,Qiuming Peng

The construction of heterojunctions provides a promising strategy to improve photocatalytic hydrogen evolution. However, how to fabricate a nanoscale TiO2/g-C3N4heterostructure and hinder the aggregation of bulk g-C3N4using simple methods remains a challenge. In this work, we use a simple in situ construction method to design a heterojunction model based on molecular self-assembly, which uses a small molecule matrix for self-integration, including coordination donors (AgNO3), inorganic titanium source (Ti(SO4)2) and g-C3N4precursor (melamine). The self-assembled porous g-C3N4nanotube can hamper carrier aggregation and it provides numerous catalytic active sites, mainly via the coordination of Ag+ions. Meanwhile, the TiO2NPs are easily mineralized on the nanotube template in dispersive distribution to form a heterostructure via an N–Ti bond of protonation, which contributes to shortening the interfacial carrier transport, resulting in enhanced electron-hole pairs separation. Originating from all of the above synergistic effects, the obtained Ag/TiO2/g-C3N4heterogenous photocatalysts exhibit an enhanced H2evolution rate with excellent sustainability 20.6-fold-over pure g-C3N4. Our report provides a feasible and simple strategy to fabricate a nanoscale heterojunction incorporating g-C3N4, and has great potential in environmental protection and water splitting.Keywords:heterojunction;Ag/TiO2/g-C3N4;Co-assembly;hydrogen evolution

研究领域: 材料科学 · 环境科学 · 光催化
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 33 ·16035-16039 · IF 3.925

An efficient hydrogen evolution photocatalyst of Rh@Cr2O3-loaded PbMoO4 twenty-six facet polyhedrons

Jing Zhang,Chunlei Li,Xingzhi Jin,Yi Zheng

Shape anisotropic semiconductors are advanced catalysts for resolving energy crises. However, modification studies are still needed to overcome their intrinsic disadvantages, such as the lack of active sites. With this aim, an excellent hydrogen evolution photocatalyst Rh@Cr2O3-loaded PbMoO4 twenty-six facet polyhedron (PM/Rh@Cr2O3) has been synthesized by a liquid method. Based on XPS, electrochemical investigation and hydrogen evolution reaction (HER) test, it is demonstrated that Rh acts as an electron collector and active site; moreover, Cr2O3 can assist Rh in the dissociation of water. In addition, Cr2O3 can also inhibit the reverse reaction of water splitting as well as the mass transfer of water. In conclusion, the H2 yield rate increased from 0 μmol g−1 h−1 of PbMoO4 (PM) to 704 μmol g−1 h−1 of PM/Rh@Cr2O3, and PM/Rh@Cr2O3 exhibited excellent photo-stability.

研究领域: 材料科学 · 能源化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2019 · IF 4.084

2D-2D heterostructured CdS–CoP photocatalysts for efficient H2 evolution under visible light irradiation

Qixiao Gai,Xiaochun Zheng,Wenjun Liu,Quanli Dong,Yingying Wang,Renxi Gao,Shoutian Ren

Visible-light photocatalytic water splitting for hydrogen evolution has attracted tremendous attention in past decades, but it still suffers from low solar-hydrogen conversion efficiency. In this paper, two-dimensional (2D) CdS was synthesized by the hydrothermal method , and 2D CoP nanosheets were synthesized by successive hydrothermal, oxidation and phosphodation process. Then 2D-2D CdS–CoP photocatalysts were formed by ultrasonically dispersing the mixed solution of CdS and CoP, and their heterostructure was confirmed by transmission electron microscopy , X-ray photoelectron spectroscopy, fluorescence spectrometer and so on. CdS–CoP with 2% CoP loading amounts exhibits a maximum photocatalytic performance of 56.3 mmolg −1 h −1 under visible light irradiation , which is 11.3 times as high as bare CdS. The enhanced photocatalytic performance of CdS–CoP should be due to the following two points: (1) high catalytic activity of CoP; (2) highly efficient separation and transfer of electron-hole pairs photogenerated in CdS due to the synthesized 2D-2D heterostructure.

CAS / MDL: 5743-04-4 10039-56-2
研究领域: 材料科学 · 能源科学
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Nanoscale · 2013 ·Vol. 6 ·期 4 ·2299-2306 · IF 6.233

Highly efficient photocatalytic hydrogen evolution of graphene/YInO3 nanocomposites under visible light irradiation

Jianjun Ding,Wenhao Yan,Wei Xie,Song Sun,Jun Bao,Chen Gao

Visible-light-driven hydrogen evolution with high efficiency is important in the current photocatalysis research. Here we report for the first time the design and synthesis of a new graphene–semiconductor nanocomposite consisting of YInO3 nanoparticles and two-dimensional graphene sheets as efficient photocatalysts for hydrogen evolution under visible light irradiation. The graphene/YInO3 nanocomposites were synthesized using a facile solvothermal method in which the formation of graphene and the deposition of YInO3 nanoparticles on the graphene sheets can be achieved simultaneously. The addition of graphene as a cocatalyst can narrow the band gap of YInO3 to visible photon energy and prolong the separation and lifetime of electron–hole pairs by the chemical bonding between YInO3 and graphene. The photocatalytic reaction with this nanocomposite reaches a high H2 evolution rate of 400.4 μmol h−1 g−1 when the content of graphene is 0.5 wt%, over 127 and 3.7 times higher than that of pure YInO3 and Pt/YInO3, respectively. This work can provide an effective approach to the fabrication of graphene-based photocatalysts with high performance in the field of energy conversion.

CAS / MDL: 16941-12-1
研究领域: 材料科学 · 能源转换 · 纳米技术
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