AICHE JOURNAL
·
2026
·
IF 4
Zhiheng Wang,Ningning Wu,Jiali Huang,Tuo Ji,Han Lin,Liwen Mu,Xiaohua Lu,Jiahua Zhu
Direct synthesis of hydrogen peroxide (DSHP) from H 2 and O 2 is indeed a promising sustainable alternative to the conventional anthraquinone oxidation process, yet achieving high H 2 O 2 productivity and selectivity simultaneously remains a significant challenge. Herein, we designed a diode-inspired interfacial microenvironment to address this challenge by synchronizing the kinetic relay of the key transport and reaction steps in DSHP. Specifically, this microenvironment was fabricated by grafting hydrophobic silane molecules onto the carbon surface followed by loading palladium nanoparticles. Results indicate that the interfacial microenvironment enables an efficient relay of H 2 dissociation, H 2 O 2 formation and desorption, shutting down the reverse path of the side reaction. Benefiting from this diode-inspired interfacial design, high H 2 O 2 productivity of 21,647.1 mol kg Pd −1 h −1 and H 2 O 2 selectivity of 93.3% were successfully achieved under ambient conditions. This work demonstrated the critical role of the interfacial microenvironment in regulating the synergy between mass transfer and reaction in heterogeneous reaction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 8.3
Baker Rhimi,Attiq Ur Rehman,Yuanzhi Hu,Sherif A. El-Khodary,Zhehao Liu,Min Zhou,Karim Harrath,Qiang Ma,Long Zhao,Zhifeng Jiang,Weidong Shi
The development of efficient and stable photocatalysts for hydrogen evolution is crucial for solar-to-fuel conversion. Here, we report Cu-porphyrin (CuTCPP)/oxygen-doped g-C 3 N 4 (O–CN) nanohybrids as high-performance sonophotocatalysts, where strong π–π stacking interactions create robust heterojunctions that promote efficient charge separation and transfer. The optimal 2 % CuTCPP/O–CN2 sample exhibited a 3.3-fold enhancement in H 2 evolution compared to O–CN2 under simulated light coupled with ultrasonication. Experimental results combined with density functional theory (DFT) calculations confirmed the suppression of charge recombination and highlighted the synergistic contribution of ultrasonic excitation with light irradiation. Furthermore, oxygen doping was found to not only reinforce the CuTCPP/O–CN interface but also provides robust anchoring sites for Pt cocatalysts, preventing leaching and aggregation while electronically modulating Pt to optimize its d-band center and H 2 adsorption free energy. These findings provide valuable insights into the rational design of stable and high-active hybrid photocatalysts for solar fuel generation.
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FUEL PROCESSING TECHNOLOGY
·
2024
·
IF 7.2
Mingkai Liu,Yang Li,Xuyun Wang,Zhongrui Gai,Qiong Rao,Tianlong Yang,Jinrui Zhang,Sanli Tang,Ying Pan,Hongguang Jin
Hydrogen energy, a promising clean source, holds potential to combat global warming. To achieve efficient and low-carbon H 2 production, we proposed an isothermal sorption-enhanced chemical looping reforming (SE-CLR) process to realize the high-purity hydrogen production and in-situ CO 2 capture at mild temperatures (550–650 °C). For practical application, the process is characterized to use Fe-Ni double metal oxide particles as steam methane reforming oxygen carriers, and K 2 CO 3 -promoted Li 4 SiO 4 particles as CO 2 sorbent. The oxygen transfer capacity of metal oxide matintained high at 57.4%, and the K-Li 4 SiO 4 absorbents remained at 22.5% CO 2 absorption capacity over 200 isothermal absorption-regeneration cycles. Conducting a synergistic conversion mechanism within double metal oxides and absorbents, and adjusting the absorbent-to-metal oxide mass ratio to 7:4, enhanced hydrogen purity to 92% and CO 2 uptake to 95%. Furthermore, in-situ CO 2 removal in CLR processes achieved methane conversion and H 2 production rates equivalent to conventional CLR processes under the same reaction conditions, but at temperatures ∼60 °C lower. The effects of the reaction temperature, pressure, steam-to-methane and methane-to-solid ratios on SE-CLR performance were studied systematically. Finally, stable hydrogen production with a purity of 91%–89% and CO 2 uptake of 94%–91% were obtained over 25 CLR cycles, with minimal changes in mechanical strength of particles.
研究领域:
能源科学
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化学工程
·
环境科学
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Science Advances
·
2021
·Vol. 7
·期 47
·
IF 14.143
Zhong Liang,Lianpeng Song,Mingzi Sun,Bolong Huang,Yaping Du
Electrochemical reduction of CO 2 (CO 2 RR) to value-added liquid fuels is a highly appealing solution for carbon-neutral recycling, especially to syngas (CO/H 2 ). Current strategies suffer from poor faradaic efficiency (FE), selectivity, and controllability to the ratio of products. In this work, we have synthesized a series of single and dual atomic catalysts on the carbon nitride nanosheets. Adjusting the ratio of La and Zn atomic sites produces syngas with a wide range of CO/H 2 ratios. Moreover, the ZnLa-1/CN electrocatalyst generates the syngas with a ratio of CO/H 2 = 0.5 at a wide potential range, and the total FE of CO2RR reaches 80% with good stability. Density functional theory calculations have confirmed that the Zn and La affect electronic structures and determine the formation of CO and H 2 , respectively. This work indicates a promising strategy in the development of atomic catalysts for more controllable CO 2 RR.
研究领域:
电化学
·
催化
·
材料科学
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环境科学
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能量转换
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2015
·Vol. 40
·期 14
·4777-4785
·
IF 3.313
Jianmin Chen,Zhang-Hui Lu,Yuqing Wang,Xiangshu Chen,Lei Zhang
In this paper, we reported a facile and effective approach for fabrication of SiO 2 –CoFe 2 O 4 supported dispersed Ag nanoparticles (NPs). The as-synthesized nanocomposites (NCs) were characterized by XRD , TEM, EDX, ICP , XPS and N 2 adsorption-desorption, and used as catalyst for H 2 production from hydrolysis of ammonia borane (AB). A poorly active catalyst of Ag NPs was dramatically converted into a highly active catalyst, in the presence of inactive SiO 2 –CoFe 2 O 4 support. Among all the Ag(0)/SiO 2 –CoFe 2 O 4 NCs catalysts tested, the Ag loading of 0.98 wt% exhibited the highest catalytic activity toward hydrolysis of AB with a highly turnover frequency of TOF = 264 min −1 at room temperature, being higher than that of most reported Ag-based catalysts. Especially, these catalysts can be readily separated from the solution for recycle purpose, and can keep the high activity even after seven times of recycle. These results showed that Ag(0)/SiO 2 –CoFe 2 O 4 NCs prepared in this study are a promising catalyst for hydrogen production from aqueous AB and for developing a highly efficient hydrogen storage system for fuel cell applications .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·Vol. 46
·期 43
·22508-22518
·
IF 5.816
Zhijun Zhang,Kezhen Chen,Jichang Lu,Qin Zou,Yuhui Zhao,Yongming Luo,Dedong He,Rongtao Li
Sn modified CuO–CeO 2 catalysts with different Sn loadings were prepared by a facile, green and solvent-free method. The effect of Sn/Ce ratio over Sn–Cu–Ce-x (x = 0, 1, 2.5, 5, 7.5) samples on CO activity and O 2 selectivity was investigated. The samples were characterized by various techniques using N 2 -adsorption/desorption, XRD , H 2 -TPR, XPS, Raman and in-situ DRIFTS . It was revealed that stronger interaction between acitve sites and support, higher amounts of Sn 2+ and Ce 3+ , associated with increased amount of oxygen vacancies , were observed on the catalyst of Sn–Cu–Ce-5. As a result, the optimized catalyst displayed an excellent catalytic performance even in the presence of CO 2 and H 2 O. In this sense, probing the Sn modified CuO–CeO 2 catalyst can elucidate some useful keys for the development of high CO 2 and H 2 O-resistance catalyst during CO-preferential oxidation in H 2 -rich streams.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2021
·
IF 8.067
Xiangchen Kong,Huiming Huang,Zhaoyang Li,Yanqin Liang,Zhenguo Li,Shengli Zhu
TiO 2 (B) nanosheets/GO (graphene oxide) hybrids are considered to be outstanding performance photocatalysts for high efficiency of H 2 evolution. However, they still suffer severe challenges during the synthetic processes, such as a large amount of the capping agents adhering on the surface and easy occurrence of aggregation. To figure out these obstacles, Ar plasma treatment as a modified method in this study not only enable the TiO 2 (B) nanosheets distributed uniformly on the GO sheets but also engineer defects within TiO 2 (B) nanosheets to significantly improve the photocatalytic activity for the water splitting. The hydrogen evolution rate of the TiO 2- x (B)/GO sheets is 1.4 times higher compared with that of original TiO 2 (B)/GO sheets without Ar plasma treatment. The improved photocatalytic properties were owing to the synergetic effects of oxygen vacancies and the heterojunction between GO and TiO 2 (B), which can promote the visible light utilization and accelerate separation and transportation of photogenerated electron-holes. This study can provide a facile pathway to prepare the two-dimensional hybrid photocatalysts with high photocatalytic H 2 activity.
研究领域:
材料科学
·
纳米科技
·
能源化学
·
光催化
·
二维材料
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BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
·
2019
·Vol. 92
·期 6
·1047-1052
·
IF 4.431
Jiang Jifei,Zhu Qiong,Guo Yu,Cheng Lin,Lou Yongbing,Chen Jinxi
Photocatalytic hydrogen production is an effective strategy for meeting energy challenges. Here, a composite for photocatalytic hydrogen production via introduction of UiO-66 nanospheres into flower-shaped ZnIn2S4 microspheres (ZIS/U6) is described. The optimum composite with 20 mg UiO-66 loading displayed the high photocatalytic rate of 1860.9 µmol g−1 h−1 with an apparent quantum efficiency of 1.4% at 420 nm under visible-light irradiation, which is nearly 3 times higher than that of ZnIn2S4. The improved photocatalytic H2 rate mainly benefited from effective electron transfer between ZnIn2S4 and UiO-66. Additionally, we tried to introduce UiO-66-NH2 and UiO-66-(SH)2 with excellent visible light absorption into ZnIn2S4 to obtain composites. Surprisingly, they did not exhibit better photocatalytic hydrogen production rates. Combined with the electrochemical test results, it was found that they had completely different electron transfer paths from ZIS/U6. Therefore, a different photocatalytic mechanism was proposed and further verified by transient photocurrent.
研究领域:
材料科学
·
化学
·
能源科学
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yunxiao Zhang,Qingxiang Cao,Xuelian Wu,Yonghao Xiao,Aiyun Meng,Qitao Zhang,Yuxiang Yu,Wei-De Zhang
Establishing effective non-platinum active sites on polymeric carbon nitride (PCN) remains a great demanding to achieve highly efficient photocatalytic hydrogen generation performance. Modification with molecular complex catalysts on PCN skeletons has been demonstrated as a promising strategy. Herein, hybrid photocatalytic material was successfully synthesized by modifying PCN with copper molecular ligand ( CuL, Schiff-based copper complex) via π-π stacking. Interestingly, atomically dispersed Cu is formed in CuL/PCN. Compared to PCN, the π-π stacking in CuL/PCN is beneficial for facilitating the migration of photogenerated electrons from PCN to CuL . Furthermore, photo-redox ability of the atomically dispersed Cu is regulated by the ligand (Schiff base) in CuL and the introduction of CuL provides abundant active sites to capture the photogenerated electrons, whereby the reductive reaction of H 2 O/H + to H 2 for CuL/PCN was significantly promoted. Consequently, an optimal hydrogen evolution rate of 15.90 μmol·h −1 was obtained on 3CuL/PCN, which was 2.02 times higher than that of 3.0 wt% Pt/PCN (7.86 μmol·h −1 ). More importantly, the hybrid material exhibits an outstanding conversion efficiency (90 %) and selectivity (99 %) for α-methylation of ketones by making full use of the in-situ generated H species and photogenerated holes under visible light irradiation.
研究领域:
材料科学
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催化
·
光化学
·
无机化学
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高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 8.3
Jingyun Mao,Chengjing Lu,Qingrong Qian,Qinghua Chen,Hun Xue,Fangyuan Cheng
Photocatalytic hydrogen evolution represents a pivotal pathway for clean energy conversion. However, the development of high-performance photocatalysts is often constrained by unsustainable synthesis methods and, more fundamentally, by the limited ability to precisely control the interfacial structure for directed charge transport. Herein, we develop a green synthesis strategy to fabricate a polyaromatic carbon layer-encapsulated TiO 2 heterojunction bridged by interfacial Ti-O-C bonds. This is achieved through the controlled calcination of biomass-derived xylose, yielding carbonaceous layers with well-defined sp 2 -hybridized configurations. The optimized Pt-2X-T300 photocatalyst demonstrates a remarkable hydrogen evolution rate of 8570.9 μmol g −1 h −1 under visible light, which is approximately 1993 times higher than that of the Pt-T300 benchmark. The enhanced performance is attributed to efficient charge carrier separation driven by the interfacial Ti-O-C bond, which optimizes the band alignment between TiO 2 and sp 2 -carbon layers. Mechanistic studies verify that the atomic-level interface establishes a rapid electron transfer pathway, yielding an apparent quantum yield of ∼8.4 % at 420 nm. This work not only establishes a methodology for converting carbohydrates into tailored carbon nanostructures but also develops a novel Ti-O-C bridged TiO 2 @carbon heterojunction architecture, offering a novel approach for designing high-efficiency solar-driven hydrogen production systems.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Lizhen Lian,Min Zhang,Liqiang Wang,You-Nian Liu
Gas–liquid–solid catalytic hydrogenation over carbon-supported catalysts is typically performed at elevated temperatures and high hydrogen pressures, primarily because hydrogen is poorly soluble in the liquid phase. Enhancing the H 2 affinity of catalysts, thereby increasing the surface coverage of active hydrogen species, is an effective strategy; however, it remains challenging. Herein, we demonstrate that the H 2 affinity of carbon-supported catalysts can be optimized by introducing metal oxides into the carbon support, thereby increasing the surface hydrogen coverage on carbon-supported catalysts and ultimately enhancing their hydrogenation performance. As a proof of concept, cobalt supported on a homogeneous composite of d-Al 2 O 3 and N-doped carbon (Co/Al 2 O 3 –NC) has been prepared. The d-Al 2 O 3 component, possessing high H 2 affinity, promotes local H 2 concentration and stabilizes the dissociated hydrogen through the formation of O–H δ+ and Al–H δ- . Consequently, Co/Al 2 O 3 –NC exhibits significantly enhanced hydrogenation performance (TOF = 343 h −1 ) across hydrogenation of p -chloronitrobenzene compared to those of Co/NC (TOF = 32 h −1 ) and Co/Al 2 O 3 (TOF = 53 h −1 ) catalysts under 100 °C and 5 bar H 2 . These findings provide new insights for designing efficient catalysts for gas–liquid–solid catalytic hydrogenation reactions over carbon-supported catalysts.
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PHYSICA B-CONDENSED MATTER
·
2026
·
IF 3.2
Junyu Huang,Di Lin,Wei Li,Bo Wang,Huiyang Xu,Zimo Wang,Yongyi Li,Shuanglong Li,Xiaorui Huang
The PCN/CdS/CdIn 2 S 4 composites exhibit excellent photocatalytic performance for H 2 evolution, H 2 O 2 production and dye degradation. • Spontaneous interfacial band bending drives a dual Z-scheme pathway to preserve highly active photogenerated charge carriers. • The superoxide radicals (.•O 2 − ) is the primary species for both continuous H 2 O 2 generation and rapid pollutant decomposition. Addressing the escalating global energy and environmental crises demands efficient, sustainable, and robust technologies. In this study, a ternary composite PCN/CdS/CdIn 2 S 4 integrating phosphorus-doped carbon nitride (PCN), cadmium sulfide (CdS), and indium cadmium sulfide (CdIn 2 S 4 ) was rationally designed via a multi-step assembly process. The optimized heterojunction exhibits outstanding performance, achieving remarkable H 2 and H 2 O 2 production rates of 7614 and 6873 μmol∙g −1 h −1 , respectively. Additionally, it demonstrates ultra-fast degradation kinetics, mineralizing 99.4% of methyl orange within just 30 min. Mechanistically, spontaneous interfacial band bending drives a dual Z-scheme charge transfer pathway. This specific energy band alignment effectively preserves strongly reducing electrons and highly oxidizing holes while significantly suppressing charge carrier recombination. Furthermore, radical trapping confirms that superoxide radicals (∙O 2 − ) are the pivotal active species, driving a two-step single-electron reduction pathway (O 2 →∙O 2- →H 2 O 2 ) for continuous H 2 O 2 generation, and coupling synergistically with localized holes for rapid organic pollutant decomposition.
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