Catalysts
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2022
·Vol. 12
·期 9
·998
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IF 4.501
Mengfan Niu,Liyun Cao,Qianqian Liu,Xiaoyi Li,Qian Chen,Dinghan Liu,Wenbin Li,Jianfeng Huang,Liangliang Feng
Exploring low-cost and highly active, cost-effective cocatalysts is of great significance to improve the hydrogen evolution performance of semiconductor photocatalysts. Herein, a novel ultrasmall V-doped NiP2nanoparticle, as an efficient cocatalyst, is reported to largely upgrade the photocatalytic hydrogen evolution reaction (HER) of g-C3N4nanosheets under visible-light irradiation. Experimental results demonstrate that V-NiP2cocatalyst can enhance the visible-light absorption ability, facilitate the separation of photo-generated electron-hole pairs and boost the transfer ability of electrons of g-C3N4. Moreover, the V-NiP2/g-C3N4hybrid exhibits prominent photocatalytic HER activity 17 times higher than the pristine g-C3N4counterpart, even outperforming the 1 wt.% platinum-loaded g-C3N4. This work displays that noble-metal-free V-NiP2cocatalyst can serve as a promising and efficient alternative to Pt for high-efficiency photocatalytic H2evolution.Keywords:g-C3N4;cocatalyst;V-NiP2;photocatalyst;hydrogen evolution reaction
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Jiayu Liao,Xiaohuan Jiang,Yingnan Duan,Huanhuan Liu,Mengkui Tian
A novel hierarchical Au/black phosphorus nanosheets/ZnIn 2 S 4 (Au/BPNSs/ZIS) heterojunction photocatalyst has been successfully synthesized in this work, in which ZnIn 2 S 4 (ZIS) nanosheets were first grown in situ on black phosphorus nanosheets (BPNSs) using the solvothermal method. Au nanoparticles were then photo-deposited on the outer surface of the ZIS. The hydrogen evolution rate of the optimal Au/BPNSs/ZIS is 1674 μmol·h −1 ·g −1 , which is 5 and 17 times higher than that of pure ZIS and few-layer BPNSs, respectively. The photocatalyst of BPNSs/ZIS is primarily attributed to the formation of Zn-P bonds between them to stabilize the connection of BPNSs/ZIS heterojunctions, according to X-ray photoelectron spectroscopy (XPS). At the same time, the work function calculation reveals that the interface electric field formed from ZIS to BPNSs is the driving force of interface charge transfer, allowing photoexcited electrons to migrate directionally on the interface and improve hydrogen evolution efficiency under visible light irradiation. Furthermore, Au nanoparticles are photo-deposited on the ZIS surface to form Schottky junctions, which improves photocatalytic performance even further. This work offers a novel approach to developing BP-based heterojunctions in photocatalysis .
研究领域:
材料科学
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光催化
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纳米技术
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能源材料
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 13.2
Aihua Yan,Bolei Hui,Liang Mao,Wenxue Zhao,Fei Huang,Zigao Su,Huaqi Yuan,Heng Wang,Nan Li,Zhiqing Xu
Utilization of active site and chemical bonding “bridge” to promote the charge transfer and expedite the catalytic kinetics has been regarded as a promising strategy to achieve highly-efficient photocatalysts. Herein, medium-entropy CdCoNiS cocatalysts coupled with ZnIn 2 S 4 matrix were prepared by a solvothermal method and subsequent water-bath treatment. The experimental results and theoretical calculation confirmed that the hydrogen adsorption capacity, charge-transfer dynamics and surface charge utilization were significantly improved due to the successful construction of dual-active sites and chemical bonding “bridge”. As a result, the optimum samples exhibited a high hydrogen evolution rate of 11.4 mmol g −1 h −1 and an apparent quantum efficiency of 11.7% at 420 nm. Moreover, the photostability was evidenced by remaining excellent photoactivity after four cycles. This work may be extended to other medium-entropy cocatalysts and provide an insight for the exploration of efficient photocatalytic hydrogen production system.
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高影响因子
APPLIED SURFACE SCIENCE
·
2026
·
IF 6.9
Hui Tang,Xiaobao Chen,Zonghan Huang,Meng Liu,Xiaoping Li,Lanxuan Wen,Yu Liu,Rongwei Li,Songjun Guo,Rongzhi Chen
Inefficiency in photogenerated charge separation, especially within the in-plane heptazine units of widely used carbon nitride semiconductors, severely restricts photocatalytic H 2 evolution. Herein, a dual electric field was constructed in a novel C 3 N 4 /C 3 N 5 /CoP (CNHJ- X /CoP) composite via the synergistic integration of a C 3 N 4 /C 3 N 5 homojunction and a C 3 N 5 /CoP Schottky junction. The optimized CNHJ-5/CoP exhibits a photocurrent density 7.5 times higher than that of pure C 3 N 5 , along with a hydrogen evolution rate of 1878 μmol·g −1 ·h −1 (apparent quantum efficiency = 14.1% at 400 nm), which is 24.5% higher than that of C 3 N 5 /CoP binary composite. X-ray photoelectron spectroscopy, density functional theory calculations, and charge dynamics characterization collectively confirm that the dual electric field enhances the in-plane charge separation efficiency within the C 3 N 5 heptazine units and facilitates the directional transfer of photoelectrons from C 3 N 5 to both C 3 N 4 and CoP. Specifically, the homojunction promotes the retention of more holes in C 3 N 5 for reaction with triethanolamine, while the Schottky junction accelerates electron transfer to CoP for H 2 evolution, thereby driving the forward reaction. This work provides new insights into the design of advanced dual-electric-field systems for enhancing charge separation in two-dimensional nanosheets, thereby boosting photocatalytic H 2 evolution.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2020
·
IF 7.183
Yanwei Sun,Chunshan Song,Xinwen Guo,Sungwon Hong,Jungkyu Choi,Yi Liu
Metal-organic framework (MOF) membranes have received increasing attention due to their unprecedented potential for energy-efficient gas separation. Compared with other MOF materials (like ZIF), fabrication and microstructural manipulation of high-performance Ti-MOF-based membranes, although being very attractive due to their excellent chemical and thermal stability, remained relatively less investigated due to the limitations of available titanium sources and heating modes. In this study, different Ti sources (TPOT, TiS 2 , and MXene) and heating modes (conventional heating, multi-mode microwave heating, and single-mode microwave heating) were examined for the preparation of NH 2 -MIL-125 membranes showing diverse microstructures and gas separation performances. The present work revealed that for the first time, MXene , the new two-dimensional Ti carbide , could be used as Ti source for synthesizing MOF membranes. The best performing NH 2 -MIL-125 membranes, which were obtained with TiS 2 as the metal source under single-mode microwave heating, exhibited the highest H 2 /CO 2 selectivity (ca. 17.2) as well as considerable H 2 permeance (1.7 × 10 −7 mol m −2 s −1 Pa −1 ), owing to an enhanced non-thermal effect of single-mode microwave heating and balanced dissolution rate of TiS 2 .
研究领域:
材料科学
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膜分离技术
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化学工程
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纳米材料
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气体分离
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可持续能源
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DOI
高影响因子
APPLIED ENERGY
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2024
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IF 10.1
Yaning Kong,Honglin Yu,Mengqi Liu,Guodong Zhang,Fei Wang
Hydrate was considered to be the next generation hydrogen storage material , and hydrate-based hydrogen storage (HBHS) would play an important role in future hydrogen economy, but sluggish hydrate formation kinetics presents huge technological challenge for its application. Herein, a nano promoter of -SO 3 − @PSNS was prepared by soap-free emulsion polymerization , and a dual kinetic promoter system (L-methionine/-SO 3 − @PSNS) was applied to enhance the formation kinetics of mixed H 2 /DIOX hydrate. At a moderate condition (12 MPa and 274.15 K), hydration efficiency under a driving force of 2.1 MPa is significantly enhanced by the synergy of the dual kinetic promoters, hydrate induction time reduces from 443.2 ± 209.73 min to 24.7 ± 17.16 min, while hydrate growth rate increases by 43.75%, and hydrogen storage capacity is up to 0.473 ± 0.041 wt% that increases by 62.8%. At a more moderate condition (10 MPa and 274.15 K) with an extremely low driving force of 0.1 MPa, enhanced hydrate formation was obtained in a composite promotion system of the dual kinetic promoters and dual thermodynamic promoters (THF/DIOX), which also performs exceptionally in term of recycling. The presence of a small amount (0.35 mol%) of THF reduces the induction time by 93.5%, and hydrate growth rate increases by 130.18%, while satisfactory hydrogen storage capacity (0.346 ± 0.017 g/g) is still remained in mixed H 2 /DIOX/THF hydrate, the structure of which was confirmed by Raman spectrum . This work presents an effect approach on enhancing the formation kinetics of H 2 -contained hydrate under low driving force, and this finding provides important insight for HBHS.
研究领域:
物理化学
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能源材料
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气体储存
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化学工程
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纳米材料科学
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分子模拟
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可持续能源
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高影响因子
Nano Select
·
2021
·Vol. 2
·期 11
·2126-2134
·
IF 0
Junwei Liang,Yuxiang Liu,Rongzheng Liu,Sufan Zheng,Zhichun Si,Duan Weng,Feiyu Kang
Preparing stable highly dispersed Pt based electrocatalyst is promising to reduce material expense of H 2 product via electrocatalytic water splitting. However, it is still a great challenge to obtain stable single atomic Pt catalysts which can be applied in acidic electrolyte. In the present work, we synthesized Pt atomic clusters on carbon quantum dots (CQDs) grafting multiwall carbon nanotube (CNT) (Pt content: 1 wt.%) catalysts and then loading the catalysts on carbon cloth (Pt content: 0.01 mg▪cm –2 ) for activity test. The overpotential of 29 mV versus RHE was obtained over 1%Pt/CQDs/CNT catalysts at the current density of 10 mA▪cm –2 , and the Tafel slope of 22 mV decade –1 was obtained, too. Especially, the catalysts showed significant stability in hydrogen evolution reactions (HER) in acidic solution, of which the overpotential was still smaller than that of 20%Pt/C after 10,000 CV cycles. CQDs provided coordinating sites for dispersing Pt atomic clusters and improved the H + concentration in adjacent area around the Pt clusters. This method provides a general strategy to design the highly efficient electrocatalysts with ultra-low precious metals for H 2 evolution in acidic electrolyte.
研究领域:
材料科学
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电化学
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纳米技术
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能量转换
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催化
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DOI
APPLIED CATALYSIS A-GENERAL
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2024
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IF 4.7
Chenyang Zhao,Yujia Liu,Yupeng Tian,Yahui Li,Junjie Feng,Wei Xu,Ning Shi,Zhe Yang,Bing Sun
Direct epoxidation of propylene (C 3 H 6 ) with hydrogen (H 2 ) and oxygen (O 2 ) over Au/TS-1 catalyst was promising way for the synthesis of propylene oxide (PO). However, high selectivity of PO (>95 %) and conversion of C 3 H 6 (>5 %) cannot be achieved at the same time. The industrialization process was severely restricted. In this paper, Au/TS-1 catalysts were synthesized by deposition precipitation method with alkali metal promoter. And alkaline gases and silane coupling post-treatment were performed to promote the catalytic activity. The prepared samples exhibited a much better C 3 H 6 conversion (6.5 %) and PO selectivity (95.1 %) compared with general catalyst using normal synthetic technology. Cs 2 CO 3 was beneficial to increasing Au nanoparticles uptake efficiency. Both NH 3 and triethoxyvinylsilane post-treatment were good for smaller and more uniform loading of Au nanoparticles. The decreasing in surface hydroxyl density effectively alleviated the occurrence of PO ring opening isomerization. The increased hydrophobicity of TS-1 surface was conducive to the rapid desorption of generated PO and significantly increased PO selectivity. Multiple pretreatment was also favorable for extending the lifetime of Au/TS-1 catalyst.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Solar RRL
·
2020
·Vol. 5
·期 6
·2000427
·
IF 7.527
Yiqun Li,Shipeng Wan,Cheng Lin,Yujie Gao,Yuan Lu,Luyang Wang,Kan Zhang
Sufficiently utilizing photogenerated electron/hole pairs for a coupled redox enables green, sustainable, and low-cost photocatalysis. Herein, a series of MoS 2 /Cd x Zn 1− x S photocatalysts with uniform 2D/2D structure are reported for solar water–reductive H 2 products coupled with the degradation of polyethylene terephthalate (PET) plastic. The MoS 2 /Cd 0.5 Zn 0.5 S heterojunction with a loading mass of 4.3 wt% MoS 2 exhibits the best H 2 evolution rate of 15.90 mmol g −1 h −1 in an aqueous solution due to its appropriate redox ability, great light absorption, and carrier separation abilities. Then, the oxidation products of PET are analyzed by 1 H-NMR spectroscopy, which demonstrates the PET being efficiently degraded to molecule compounds, such as formate and acetate. The work provides a feasible solution to the problem of plastic pollution and meets the demand for sustainable clean energy simultaneously.
研究领域:
材料科学
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环境科学
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能源科学
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化学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124243
·
IF 7.5
Yuanyuan Xu,Yunhua Lu,Pengwei Lv,Guoyong Xiao,Tonghua Wang,Lin Li
Interfacial defects between fillers and polymer matrix restrict the separation performance of mixed matrix membranes (MMMs). Herein, low-order polyimide (PI)-based covalent organic frameworks (COFs) fabricated from 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT) and pyromellitic dianhydride (PMDA) were firstly adopted as fillers to modify thermally rearranged (TR) membranes. Distinct from highly crystalline COFs, low-order PI-COFs contain more exposed terminal reactive groups. These functional groups can form covalent linkages with poly(amic acid) precursors, which effectively suppresses the generation of non-selective interfacial voids and improves the interfacial compatibility between filler and polymer matrix. The hierarchical pores of PI-COFs construct low-resistance gas transport pathways, and triazine/imide polar sites deliver strong affinity for CO 2 . After thermal rearrangement at 450 °C, TR/COFs-2.3 achieves drastically boosted permeabilities: 4632 Barrer (CO 2 ), 3867 Barrer (H 2 ), 795 Barrer (O 2 ) and 215 Barrer (N 2 ). Its CO 2 /N 2 selectivity slightly increases to 21.54, while O 2 /N 2 and H 2 /N 2 selectivities moderately decline to 3.70 and 17.99. This membrane exceeds the 2008 Robeson upper bound for H 2 /N 2 , and nearly reaches the limit for CO 2 /N 2 and O 2 /N 2 . It also displays improved long-term aging stability (66–74% permeability retention after 180 days, versus 52% for neat TR membrane) and stable performance in a 6-day continuous mixed-gas test. This work proposes a low-order COF interfacial modification strategy to alleviate interfacial defects, providing a practical route to prepare high-performance TR-based MMMs.
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高影响因子
JOURNAL OF CATALYSIS
·
2026
·
IF 6
Xu Chen,Weijing Cao,Ziyi Fan,En Zhao,Lang Zhou,Zupeng Chen
AuPd-TCN enables photocatalytic 5-HMF oxidation coupled with H 2 evolution. • Achieving 69.2% DFF yield and 421.9 μmol·g⁻ 1 ·h⁻ 1 H 2 evolution rate within 2 h. • Revealing AuPd-TCN interfacial interactions to promote charge separation and transfer. • Confirming valence-band oxidation and conduction-band reduction coupling by DRIFTS and EPR. The selective oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-diformylfuran (DFF) coupled with hydrogen (H 2 ) evolution offers a sustainable strategy for the high-value conversion of biomass-derived platform chemicals and clean energy production. In this study, tubular carbon nitride (TCN) is first prepared via self-assemble of a supramolecular precursor, followed by the loading of AuPd bimetallic nanoparticles on its surface through an impregnation-reduction method to construct the AuPd-TCN photocatalyst. Under visible-light irradiation for 2 h, AuPd-TCN delivers a DFF yield of 69.2% and a H 2 evolution rate of 421.9 μmol·g −1 ·h −1 , markedly outperforming pristine TCN (22.4%, 17.7 μmol·g −1 ·h −1 ), Au-TCN (39.8%, 204.2 μmol·g −1 ·h −1 ), and Pd-TCN (48.6%, 255.4 μmol·g −1 ·h −1 ). Structural and photoelectrochemical characterizations reveal that Au and Pd form bimetallic nanoparticles on TCN with strong interfacial electronic interactions that promote the separation and transfer of photogenerated charge carriers. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirms that the hydroxymethyl group of 5-HMF is selectively oxidized to an aldehyde group, while the furan ring skeleton remains intact during the reaction. Active species trapping experiments and electron paramagnetic resonance (EPR) analysis further demonstrate that photogenerated holes (h + ) and electrons (e - ) are the primary active species in this coupled reaction: h⁺ drives the selective oxidation of 5-HMF to DFF, while e - reduces H⁺ to H 2 on the AuPd bimetallic nanoparticles surface. This study provides an effective strategy for simultaneous biomass-derived chemical valorization and clean hydrogen production. Download: Download high-res image (147KB) Download: Download full-size image
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Hong Tian,Jiwen Fu,Lei Liu,Hongyu Chen,Zheng Zeng,Sijin Chen,Fubin Ma
With moderate N content and rich micropore, NC-AC shows the highest CO 2 uptake. • N-doping and pore structure control low/high-pressure CO 2 sorption, respectively. • Optimal pore size for CO 2 adsorption increases with adsorption pressure. • Pyrrolic N exhibits the most significant enhancement in CO 2 adsorption. In steam methane reforming (SMR) for hydrogen production, efficient CO 2 removal is essential. Although ultra-micropores and nitrogen doping enhance CO 2 adsorption on carbon adsorbents, their combined effects under high-pressure conditions remain unclear. Herein, a nitrogen-doped biochar (NC), an activated biochar (AC), and a nitrogen-doped activated carbon (NC-AC) were prepared from waste coconut shell. AC exhibited a highly developed pore structure (specific surface area of 1755 m 2 /g and micropore volume of 0.644 cm 3 /g), whereas NC was rich in nitrogen content (16.49 wt%). NC-AC combined a moderate nitrogen content (3.06 wt%) with an abundant porous network. High-pressure CO 2 adsorption isotherms revealed a pressure-dependent evolution in the relative contributions of nitrogen-containing functional groups and pore structure: the contribution of nitrogen-containing functional groups was more pronounced at low pressures (<0.5 bar), the contribution of pore structure gradually increased at intermediate pressures (0.5–2 bar), and pore structure played a more pronounced role at high pressures (>2 bar). Dynamic column breakthrough experiments with a CO 2 /H 2 mixture (20/80 vol%) demonstrated that NC-AC exhibited the highest CO 2 uptake. Molecular simulations showed that at low pressure, the 0.6 nm pore exhibited the highest CO 2 adsorption, while at 10 bar, the 0.8 nm pore surpassed due to its strong interaction forces and large packing space. In the 0.8–1.0 nm pores, CO 2 preferentially formed multilayer adsorption near the pore walls and pushed H 2 toward the pore center. Among nitrogen-functional groups, pyrrolic N (N-5) significantly enhanced the CO 2 adsorption capacity and selectivity. Download: Download high-res image (94KB) Download: Download full-size image
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高影响因子
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