CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jia Shen,Qian Xiang,Yake Lou,Jiajie Ye,Yanglong Guo,Wangcheng Zhan,Li Wang,Xiao-Ming Cao,Aiyong Wang,Xuan Tang,Yun Guo
The preferential oxidation of carbon monoxide (CO-PROX) in rich hydrogen is a highly appealing technology for removing trace amounts of CO in hydrogen purification. Nevertheless, the requirements for realizing both a wide optimal working temperature range and high stability under industrial operating conditions remain a significant challenge. Here, we proposed a strategy for designing robust PtFe bifunctional catalysts stabilized by silanol nests on dealuminated Beta zeolite. The silanol nests formed upon dealumination effectively anchored Fe species, which subsequently facilitated the co-localization of Pt with the Fe sites. As a result, highly dispersed Fe species were stabilized in conjunction with Pt ensembles, achieving 100 % CO conversion within a wide working temperature range of 25 °C to 180 °C. Furthermore, this catalyst also demonstrates exceptional stability, maintaining 100 % CO conversion over 72 h of continuous CO-PROX operation under industrially relevant conditions (80 °C, in the presence of H 2 O and CO 2 ). Mechanistic investigations revealed that the high efficiency of O 2 utilization on the highly dispersed PtFe nanoparticles on dealuminated Beta zeolite not only promotes activity but also enhances stability for the CO-PROX reaction.
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DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Zhenwen Yang,Ziyi Shui,Mengfei Zhao,Zheng Wei,Fenglian Zhang,Xiaoxiao Duan,Ben Niu,Bingzhi Li,Guoxia Jiang,Zhengping Hao
Catalytic NH3 decomposition has drawn growing interest in constructing the NH3-based hydrogen economy. Ni catalysts show great potential in this reaction but suffer from low atom utilization efficiency and unclear structure–activity relationship. Here, atomic layer deposition was used to grow Ni clusters on CeO2 nanorods to create a highly active catalyst for NH3 decomposition, which outperforms the conventional Ni nanoparticle catalysts and the synthesized Ni single-atom catalyst. The distinct catalytic behaviors of Ni clusters and Ni single atoms were systematically investigated. It is revealed that the interfacial confinement effect induces a strong electronic interaction between Ni clusters and CeO2, wherein abundant Ov-Ce3+ sites are formed in the vicinity of Ni clusters, resulting in interfacial electron-enriched Niδ− sites. These Niδ− sites bind to N adatoms moderately, favoring N–H bond cleavage and nitrogen desorption (the rate-determining step), which is the origin of the high activity. In contrast, ionic Ni single atoms diffusing into the CeO2 lattice display a much lower activity since strongly bound N adatoms block the active sites and retard the overall rate. This work provides a deep understanding of Ni-catalyzed NH3 decomposition and paves the way for designing high-performance metal catalysts for other structure-sensitive reactions.
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
Nature Communications
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2025
·Vol. 16
·期 1
·1-12
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IF 15.7
Fu Hui,Wu Yaqiang,Guo Yuhao,Sakurai Takuya,Zhang Qianqian,Liu Yuanyuan,Zheng Zhaoke,Cheng Hefeng,Wang Zeyan,Huang Baibiao,Wang Qian,Domen Kazunari,Wang Peng
Solar-driven photocatalytic water splitting offers a sustainable pathway to produce green hydrogen, yet its practical application encounters several challenges including inefficient photocatalysts, sluggish water oxidation, severe reverse reactions and the necessity of separating produced hydrogen and oxygen gases. Herein, we design and develop a photocatalytic system composed of two separate reaction parts: a hydrogen evolution cell containing halide perovskite photocatalysts (MoSe 2 -loaded CH(NH 2 ) 2 PbBr 3-x I x ) and an oxygen evolution cell containing NiFe-layered double hydroxide modified BiVO 4 photocatalysts. These components are bridged by a I 3 − /I − redox couple to facilitate electron transfer, realizing efficient overall water splitting with a solar-to-hydrogen conversion efficiency of 2.47 ± 0.03%. Additionally, an outdoor scaled-up setup of 692.5 cm 2 achieves an average solar-to-hydrogen conversion efficiency of 1.21% during a week-long test under natural sunlight. By addressing major limitations inherent in conventional photocatalytic systems, such as the cooccurrence of hydrogen and oxygen in a single cell and the resultant severe reverse reactions from hydrogen and oxygen recombination, this work introduces an alternative concept for photocatalytic system design, which enhances both efficiency and practicality.
研究领域:
材料科学
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能源科学
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环境科学
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DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Qiqi Gu,Shijin Cheng,Qiaoyi Xiao,Qianchen Ou,Hongmei Wang,Yuan Lian,Liping Guo
The FeCo-LDH/Cd 1-x Zn x S nanocomposite was synthesized via an impregnation method, employing FeCo-LDH as a cocatalyst for simultaneous upcycling of polyethylene terephthalate (PET) plastics and photocatalytic hydrogen production. The 5 %LDH/Cd 0.5 Zn 0.5 S nanocomposite demonstrated an optimal hydrogen evolution rate of 3.67 mmol·g −1 ·h −1 in alkaline PET solution, which is 2.3 times higher than pristine Cd 0.5 Zn 0.5 S. Notably, the photocatalyst retained stable performance over six recycling tests without significant activity loss. Concurrently, PET oxidation by photogenerated holes yielded acetate as the primary product, achieving an 87 % yield. The real-world applicability of this approach was further validated through the successful photoreforming of a PET bottle. UV–vis DRS, TRPL, and PEC analyses revealed that the incorporation of appropriate amount of FeCo-LDH significantly enhanced charge carrier separation, thereby boosting the photocatalytic activity. Furthermore, UPS and DFT calculations elucidated the mechanistic pathway for PET conversion and hydrogen production over FeCo-LDH/Cd 0.5 Zn 0.5 S. This study presents a promising strategy for co-producing hydrogen and value-added chemicals from PET waste, highlighting its potential for practical recycling applications.
研究领域:
材料科学
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环境科学
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能源化学
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DOI
高影响因子
Frontiers of Chemical Science and Engineering
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2023
·Vol. 18
·期 1
·1-9
·
IF 4.5
Sun Likun,Xiong Kesi,Zhang Baoning,Fang Jinghong,He Yingchao,Wang Min,Gan Zhixing,Du Fanglin,Sun Qiong,Yu Liyan,Dong Lifeng
In a dual-chamber photocatalytic fuel cell device, polyvinyl alcohol degradation and H 2 evolution were concurrently achieved. The setup involved commercial P25 as the photoanode and Ag@Fe 2 O 3 nanoparticles as the cathode. Additionally, the feasibility of a Fenton-like reaction in the cathode, utilizing Fe 2+ ions and pumped O 2 , was demonstrated. Different cathode materials, polyvinyl alcohol types, and pH values’ effects were assessed on device performance. Quenching tests highlighted photoinduced holes (h + ) and OH· radicals as pivotal contributions to polyvinyl alcohol degradation. Long-term stability of the device was established through cycling experiments.
研究领域:
环境科学
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材料科学
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能源科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Yuanli Li,Chunqiang Zhuang,Shi Qiu,Junfeng Gao,Quan Zhou,Zaicheng Sun,Zhenhui Kang,Xiaodong Han
Metal halide perovskites with broad optical absorption and long carrier lifetime are considered as ideal photocatalysts. However, their poor stability in water greatly impedes their application in photocatalytic H 2 evolution because they lose their crystalline structure in water. Herein, we proclaim a new class of photocatalysts: all-inorganic Cs-Cu-Cl perovskite quantum dots (QDs). It exhibits a high photocatalytic hydrogen production rate of ∼ 3.1 mmol/g/h without any cocatalyst under AM 1.5-G solar irradiation (100 mW/cm 2 ). Especially, it remains the high activity for up to 330 h without apparent deterioration of the hydrogen production rate. Density functional theory (DFT) calculations reveal that the Cu site works as the electron and proton absorption sites as the H 2 production active center. To our best knowledge, there is no report of metal halide perovskites as water-stable photocatalysts. This work opens an innovative way for guiding the exploration of metal halide perovskites photocatalysts for stable photocatalytic H 2 evolution.
研究领域:
材料科学
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能源科学
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化学
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DOI
高影响因子
Nano Energy
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2023
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IF 17.6
Kailai Zhang,Xiaodong Sun,Haitang Wang,Yali Ma,Hongwei Huang,Tianyi Ma
Single component semiconductor materials with piezoelectric response can promote the activation of hydrogen ions (H + ) and the generation of hydrogen (H 2 ) under the action of mechanical force, but the high recombination rate of carriers is the major obstacle to strengthen piezocatalytic efficiency. Here, a groundbreaking Bi 2 MoO 6 -BaTiO 3 (BMO-BTO) Type-I heterojunction piezocatalyst is successfully fabricated through a solvothermal strategy, and applied for cocatalysts-free piezocatalytic H 2 production reaction. Under ultrasonic vibration, the H 2 production rate of BMO-0.1BTO heterojunction can reach up to nearly 152.57 µmol/g/h, which is approximately 9.33 and 4.47 times with respect to that of pristine BMO (16.36 µmol/g/h) and BTO (34.16 µmol/g/h) alone, respectively. Furthermore, BMO is also combined with other commonly used piezocatalysts to construct heterojunctions, and analogous marvelous piezocatalytic H 2 production performance was attained. The enhanced piezocatalytic H 2 production performance can be credited to the established built-in electric field (BIEF) in heterojunction extraordinarily suppressed the recombination rates of piezocarriers, rather than an increase in piezoelectricity, which is emphatically verified through a series of physics and chemical characterizations. This study presents an innovative paradigm for fabricating BMO-based heterojunction piezocatalyst to efficiently convert mechanical energy into chemical energy.
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
MACROMOLECULES
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2025
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IF 5.2
Fan Hu,Jinpeng Luo,Shichao Feng,Liangqiang Wei,Shinji Ando,Yinhua Wan,Yongbing Zhuang
Conventional polyimide (PI) membranes exhibit low H2/CO2 selectivity (≤3.1). To address this limitation, this study synthesized a novel diamine monomer, 5-amino-2-(4-hydroxy-3-aminobenzene)-benzoxazole (OH-BOA), specifically designed with benzoxazole and hydroxyl functionalities. Subsequently, OH-BOA and its structural counterpart 5-amino-2-(4-hydroxy-3-aminobenzene)-benzimidazole (OH-BIA) were copolymerized with pyromellitic dianhydride (PMDA) to yield four hydroxy-functionalized poly(benzoxazole-benzimidazole-imide)s (OH-CoPIs). These OH-CoPIs exhibited good solubility, robust mechanical properties (tensile strength ≥ 114.9 MPa), high glass transition temperatures (Tg > 400 °C), and low coefficients of thermal expansion (CTE ≤ 28.3 ppm/K). Notably, they achieved a significantly enhanced H2/CO2 selectivity of up to 12.2, surpassing the commercial Matrimid 5218 (3.1) by 4-fold. Systematic evaluation revealed that increasing benzoxazole content reduced the CTE while enhancing tensile strength, Young’s modulus, and H2/CO2 selectivity. The thermally rearranged membrane (TR-40CoPI-400, 400 °C) achieved high H2 permeability (26.00 Barrer) with optimal selectivity (7.6) and exceptional CO2 plasticization resistance. The synergistic integration of benzimidazole, benzoxazole, and hydroxyl groups enables high-performance PI membranes for H2/CO2 separation.
研究领域:
高分子材料科学
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膜分离技术
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气体分离
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功能高分子
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能源材料
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DOI
高影响因子
ChemSusChem
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2025
·
IF 6.6
Yanmei Zheng,Qichao Chen,Jianghong Ouyang,Ziwei Hang,Zupeng Chen
The simultaneous photocatalytic production of hydrogen peroxide (H 2 O 2 ) and hydrogen (H 2 ) from water has received widespread attention. However, the inherent inefficiencies in dynamic processes, such as sluggish charge separation or accumulation, pose substantial limitations to overall photocatalytic performance. Here, a manganese-assisted carbon nitride/carbon nanoribbons (CN/CT-Mn) heterojunction is developed via a straightforward thermal evaporation process. The optimized CN/CT-Mn photocatalyst demonstrates exceptional activity for concurrent H 2 O 2 and H 2 production under ambient conditions, achieving impressive yields of 104 and 720 μmol g −1 h −1 , respectively. The enhanced performance can be attributed to the enhanced charge separation and the regulation of electron reduction kinetics resulting from the construction of the heterojunction interface. Notably, the presence of Mn atoms introduces an additional impurity level, enabling precise control over the reduction selectivity of photogenerated electrons. Graphical Solar-driven dual production of H 2 and H 2 O 2 is achieved via an Mn-doped carbon nitride/nanoribbon heterojunction. The built-in electric field at the heterojunction interface directs electron transfer from CN to Mn-CT, while Mn atoms enhance proton adsorption, selectively boosting H 2 evolution.
研究领域:
材料科学
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光催化
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能源化学
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纳米材料
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环境科学
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DOI
PubMed
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Yongtao Zhang,Zaizheng Jiang,Zhihe Xin,Qingqi Dong,Fei Wang
Traditional coal burning emits a large amount of pollutants, including sulfur dioxide (SO2), nitrogen oxides, and carbon dioxide (CO2), severely contaminating the environment and exacerbating global warming. In contrast, integrated gasification combined cycle (IGCC) technology, with highly efficient and clean characteristics, significantly reduces pollutant emissions and has a positive impact on environmental protection. It is a simple and effective method to obtain hydrogen (H2) by purifying IGCC fuel gas with the main components of H2 and CO2. Thermodynamic promoter tetra-n-butyl ammonium bromide (TBAB) is widely used in gas separation of IGCC fuel gas by the hydrate method. In this work, polystyrene nanoparticles grafted by –SO3– groups (−SO3–@PSNS) and grafted by –SO3– groups and Ag particles (Ag&–SO3–@PSNS) are used together with TBAB, respectively, to promote the formation of hydrate. The gas separation effect and growth morphology are studied. The experimental results demonstrate that the incorporation of nanopolymer can significantly enhance the separation efficiency (SFr) of a mixture of H2 and CO2. Notably, compared to the reaction solution without nanopolymer, 2 mmol/L –SO3–@PSNS exhibits the most pronounced effect on gas separation, resulting in an impressive gas consumption of 0.755 ± 0.323 mmol/L and a remarkable increase in the separation factor (SF) by 106%. After loading silver nanoparticles, the promoting effect of Ag&–SO3–@PSNS is further strengthened. Under Ag&–SO3–@PSNS-20%, the gas consumption reaches the maximum of 0.775 ± 0.003. Under Ag&–SO3–@PSNS-30%, the SF rises from 32.79 ± 6.27 to 37.92 ± 7.19, indicating an impressive increment of 15.80%. The visualized droplet experiment shows that Ag&–SO3–@PSNS significantly promotes the nucleation of hydrate and the growth rate of hydrate.
研究领域:
能源与燃料
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环境科学
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化学工程
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纳米技术
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DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Qingguo Yu,Yimin Liu,Qingru Zeng,Yuxiang Yang,Shunyan Ning,Yuezhou Wei,Xinpeng Wang,Deqian Zeng
Photocatalytic technology provides key benefits in utilizing solar energy for H 2 production and pollutant removal, making the pursuit of efficient photocatalysts a vital area of focus. Herein, a novel p-n heterojunction photocatalyst was synthesized by loading ZnSe nanoparticles onto Cu 2−x Se nanoplates, creating an internal electric field that facilitates the efficient separation of charge carriers and significantly enhances photocatalytic activity. The 14 % Cu 2−x Se/ZnSe nanocomposite exhibits excellent photocatalytic performance, achieving an H 2 production rate of 1846 μmol·g −1 ·h −1 , roughly 34 times that of pure ZnSe. Additionally, the Cr(VI) reduction rate constant of nanocomposite was 0.0277 min⁻¹ , which is 20 times and 5 times higher than those of ZnSe and Cu 2−x Se, respectively. The Cu 2−x Se/ZnSe photocatalyst demonstrated exceptional stability and reusability during multiple cycles of H 2 production and Cr(VI) reduction. An in-depth examination of experimental data and density functional theory (DFT) calculations led to proposing a potential mechanism. This work introduces a simple synthesis method for ZnSe-based photocatalysts, offering a novel approach for the effective application of solar energy in environmental and energy fields.
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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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Changkun Qiu,Hao Zhang,Qingrun Li,Yifan Song,Fei An,Haozhi Wang,Shiqiang Wang,Liang Zhu,Chunxiao Lv,Dongzhi Zhang
To enhance the detection performance of hydrogen (H 2 ), we employed a self-sacrificing template method to prepare a three-dimensional (3D) PdCu-modified Ti 3 C 2 T x nanocomposite , denoted as PdCu/Ti 3 C 2 T x . Within 3D PdCu/Ti 3 C 2 T x nanocomposite, PdCu as the active center component, was evenly distributed on Ti 3 C 2 T x nanosheets . The unique architecture increased the exposure of active center sites, while the Ti 3 C 2 T x nanosheets provided additional gas diffusion channels, thereby contributing to improved gas sensing performance. Comparing to PdCu nanoparticles , PdCu/Ti 3 C 2 T x exhibited an enhancing response and a fast response time of 4 s to 0.5 % H 2 . PdCu/Ti 3 C 2 T x also showed an ultra-low detection limit of 0.1 % H 2 and excellent repeatability, selectivity and long-term stability. The outstanding gas sensing performance could be attributed to the 3D structure and the heterostructure between PdCu and Ti 3 C 2 T x . The insights gained from this study provide novel perspectives for designing and synthesizing high-performance gas-sensitive materials.
研究领域:
材料科学
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化学传感器
·
纳米技术
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DOI
高影响因子
危险品化学品经营许可证（带存储）