PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2025
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IF 2.9
Qianqian Peng,Chengxuan Zhou,Shucan Qin,Jinbiao Liang,Shengyun Xu,Jiaming Mao,Jianming Shi,Yanrong Liu,Yunqian Ma
Electrochemistry allows for the simultaneous conversion of hydrogen sulfide (H2S) to hydrogen (H2) and sulfur, achieving atomic economy, and is a sustainable and cost-effective method. At the same time, an electrolyte with high conductivity and H2S absorption that can effectively capture H2S in an electrochemical process is essential. An ionic liquid electrolyte system for the absorption and electrolysis of H2S was constructed using the guanidine salt ionic liquid with amine-based functional groups as the carrier electrolyte, water as the solvent, and NaOH as the H2S absorber. The prepared electrolyte ([TMG][IM]-AE-30) showed a strong absorption of H2S with an equilibrium solubility of 100.82 g L−1. Under constant potential electrolysis at 1.0 V vs. RHE, the maximum hydrogen production rate reaches 2919.97 μmol h−1 and the Faraday efficiency reaches 99%, and the anodic product is α-sulfur with a production of 0.881 g after electrolysis for 8 h; the current density and hydrogen production rate are still higher than those of the AE systems after three cycles. Overall, the system has good hydrogen sulfide absorption and electrolysis performances, and [TMG][IM] can effectively improve the H2S absorption and electrolysis efficiencies.
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高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2025
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IF 6.2
Wang Lu,Mingwei Xia,Ziyue Tang,Yingquan Chen,Xianhua Wang,Haiping Yang,Hanping Chen
Poly-generation of porous char and H 2 -rich syngas is a key technology for the full and high-value use of carbon and hydrogen elements in biomass. In this study, the synergistic evolution and regulation mechanisms of H 2 and porous carbon during K-assisted bamboo gasification were investigated using fixed-bed pyrolysis-gasification system. The results show that, due to steam activation, both the H 2 production rate and the physicochemical properties of char initially increase and then decline with prolonged gasification time, reaching their peak in the middle stage of the process. The hydrogen conversion rate further indicates that partial gasification achieves higher production efficiency, which is favorable for the poly-generation. K accelerates the evolution of both char and H 2 , enhancing their quality and ultimately enabling the poly-generation of 31.5 mmol/g H 2 and porous carbon with a S BET of 1917 m 2 /g. Moreover, K promotes oxygen enrichment in char, particularly the incorporation of O=C-OR and C=O groups on the char surface, thereby improving the functional applicability of the carbon.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Ziheng Li,Shenghan Ji,Fengting Yao,Yan Dai,Xuehua Ruan,Xiaobin Jiang,Wenji Zheng,Gaohong He
Covalent organic frameworks (COFs) are regarded as disruptive membrane materials owing to their versatile functionalities, high stability and ordered nanochannels. However, a major obstacle to the application of COF-based membranes in gas separation is the inherent size difference between their pore sizes and target gas molecules. Herein, we employed a confined cross-linking strategy to graft CO 2 -philic poly-ethyleneimine (PEI) onto carboxylic acid-type iCOF membranes, constructing a gradient wedge-shaped pore wall structure to enhance H 2 separation. High-density carboxyl group-containing iCOF nanosheets were prepared via an improved single-phase solution method and assembled into membranes. 1-ethyl-3-(3-dimethylami-nopropyl) carbodiimide/N-Hydroxysuccinimide (EDC/NHS) coupling chemistry was used to functionalize iCOF membranes with PEI. The introduction of a large number of amino groups via PEI enhances CO 2 adsorption by 81.4%. Meanwhile, the grafting of PEI reduces defects or pinholes on the membrane surface and improves the mechanical properties and stability. As a result, the PEI-functionalized iCOF@PEI-4 membrane exhibits a H 2 permeance of 1103 GPU and an H 2 /CO 2 selectivity of 21.3, positioning its performance among advanced membranes and surpassing the 2008 Robeson upper bound. Customized structural design of iCOF membranes through tailored functionalization may provide insights for designing molecularly selective COF membranes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Kai Deng,Qiqi Mao,Wenxin Wang,Peng Wang,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Seawater splitting is considered as a promising way to replace water splitting for H 2 production due to the enrichment of seawater resources. However, the development of this technology has been greatly hampered by the lack of efficient electrocatalysts and the detrimental effects of chlorine electrochemistry. Herein, we report a defect-rich low-crystalline Rh metallene ( l -Rh metallene) with an amorphous/crystalline hetero-phase structure for seawater electrolysis, where chlorine generation is avoided by replacing the oxygen evolution reaction (OER) with the hydrazine oxidation reaction (HzOR). Benefiting from the large surface-to-volume ratio, abundant active sites and unique electronic structure, the l -Rh metallene exhibits out-standing catalytic activity for both hydrogen evolution reaction (HER, −38 mV at 10 mA cm −2 ) and HzOR (−2 mV at 10 mA cm −2 ). Notably, an ultra-low voltage of only 28 mV is required to achieve 10 mA cm −2 in two-electrode hydrazine-assisted seawater splitting system.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Xiaofan Liu,Lina Kong,Jianping Xu,Ziyu Lin,Danhao Xu,Jiawei Sun,Shaobo Shi,Xiaosong Zhang,Lan Li
Photothermal catalysis (PTC) water splitting outperforms traditional photocatalysis, but understanding of the photothermal/photochemical coupling mechanism is limited, hindering improvements in solar energy conversion efficiency. We grafted NiS ultrafine nanoparticles on hydrothermal-prepared ZnIn 2 S 4 nanosheet film via a photo-deposition process. Metallic NiS acts as photothermal/photochemical active sites and enhances solar light absorption and carrier separation of ZnIn 2 S 4 , achieving 41.14% photothermal conversion efficiency. The NiS/ZnIn 2 S 4 film exhibits a high and stable PTC H 2 production rate of 31.19 mmol·m -2 ·h -1 , which was 7.1 and 3.8 times higher than that of the pristine ZnIn 2 S 4 and the Pt/ZnIn 2 S 4 film with the same cocatalyst content, respectively. Photothermal, PTC, photoelectrical testing and DFT calculations demonstrate that the photothermal effect and synergistic photothermal/photochemical coupling contribute to the high PTC performance of NiS/ZnIn 2 S 4 . Thermodynamically, the increased temperature of NiS/ZnIn 2 S 4 enhances carrier generation and reduces Gibbs free energy (ΔG H ) for H 2 adsorption/desorption. Kinetically, temperature gradients at macro and micro levels enhance H 2 diffusion and electron convergence near NiS. This investigation of photothermal catalysis synergy provides promising strategy for designing efficient solar-to-hydrogen energy conversion systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Min Chen,Xubo Huang,Chen Chen,Wenqing Hou,Yiming Xu
Production of H 2 from water splitting is challenging. Herein, we report an increased production of H 2 on Zn 0.5 Cd 0.5 S (ZnCdS) in aqueous solution under a 420 nm LED lamp, via 4 wt % MCo 2 O 4 (M = Mg, Cr, Mn, Fe, Co, Ni, Cu, and Zn). Without addition of sacrifices, the rate of H 2 evolution ( R H , in a unit of mmol g ―1 h ―1 ) was 0.0154 for ZnCdS, and 0.057―0.551 for MCo 2 O 4 /ZnCdS. On addition of Na 2 S/Na 2 SO 3 , the corresponding R H increased to 18.5 and 31.5―78.2, respectively. In both cases, no H 2 was observed for MCo 2 O 4 . However, the R H obtained in presence of Na 2 S/Na 2 SO 3 had a negative correlation with M s and R 2 , respectively, where M s was the magnetization degree of MCo 2 O 4 , and R 2 was the charge transfer resistance for MCo 2 O 4 /ZnCdS at solid-liquid interface. Electrochemical measurement showed that MCo 2 O 4 /ZnCdS was more active than ZnCdS for proton reduction, water oxidation, and water(sulfide/sulfite) photo-oxidation, respectively. According to the solid photoluminescence, band parameters, and open circuit potentials, formation of a p-n junction is proposed, which facilitates the photoelectron transfer to ZnCdS for proton reduction, and the photohole transfer to MCo 2 O 4 for water (sulfide/sulfite) oxidation. It is also proposed that the magnetic field of MCo 2 O 4 inhibits the charge transfer between MCo 2 O 4 and ZnCdS. This work suggests that MCo 2 O 4 spinels are good co-catalysts, but their magnetization need to be minimized.
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Nature Chemistry
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2024
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IF 19.2
Zhang Yangyu,Peng Xuanbei,Tian Han-Rui,Yang Bo,Chen Zuo-Chang,Li Jiejie,Zhang Tianhua,Zhang Mingyuan,Liang Xiaocong,Yu Zhiyang,Zhou Yanliang,Zheng Lirong,Wang Xiuyun,Zheng Jian-Wei,Tang Yu,Au Chak-tong,Jiang Lilong,Xie Su-Yuan
Developing highly effective catalysts for ammonia (NH 3 ) synthesis is a challenging task. Even the current, prevalent iron-derived catalysts used for industrial NH 3 synthesis require harsh reaction conditions and involve massive energy consumption. Here we show that anchoring buckminsterfullerene (C 60 ) onto non-iron transition metals yields cluster-matrix co-catalysts that are highly efficient for NH 3 synthesis. Such co-catalysts feature separate catalytic active sites for hydrogen and nitrogen. The ‘electron buffer’ behaviour of C 60 balances the electron density at catalytic transition metal sites and enables the synergistic activation of nitrogen on transition metals in addition to the activation and migration of hydrogen on C 60 sites. As demonstrated in long-term, continuous runs, the C 60 -promoting transition metal co-catalysts exhibit higher NH 3 synthesis rates than catalysts without C 60 . With the involvement of C 60 , the rate-determining step in the cluster-matrix co-catalysis is found to be the hydrogenation of *NH 2 . C 60 incorporation exemplifies a practical approach for solving hydrogen poisoning on a wide variety of oxide-supported Ru catalysts.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Jiamin Li,Shenghong Li,Shihao Lu,Xuhui Geng,Yafeng Guan
A micron-scale bilayer sensor was fabricated in situ by electrohydrodynamic jet printing for detecting H 2 gas with highly selectivity, sensitivity and stability. The sensor consisted of a Pt loaded mesocellular silica foam (Pt-MCF) catalytic filter layer, and a ZnO/SnO 2 /Au (ZSA) sensing layer. Benefiting from the selective catalytic oxidation for CO in the catalytic filter layer, the cross-interference of CO on this sensor was reduced from 58 % to 15 %. The sensor also demonstrated a satisfactory selectivity to H 2 in interfering gases of CO 2 and CH 4 due to its high specific response to H 2 . In the ZSA sensing layer, the n-n heterojunction (ZnO-SnO 2 ) and abundant active sites on the Undaria pinnitafida -like curved nanosheet structure effectively enhanced the response of H 2 by 6.7 times. The sensors exhibited a wide H 2 dynamic range of 0.5–500 ppm with low detection limit of 94 ppb. The response/recovery time to 50 ppm H 2 was 24 s/35 s. The sensor also showed good long-term stability in 28-day response-repeatability measurement (RSD=5.3 %) and good anti-humidity.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jing Wang,Xingyu Niu,Qi Hao,Kun Zhang,Xinyi Shi,Liping Yang,Hui Ying Yang,Jilei Ye,Yuping Wu
Low charge separation efficiency significantly hampers the performance of photocatalytic hydrogen production. Constructing heterojunctions emerges as a crucial strategy to enhance photocatalytic activity by improving charge separation. An S-scheme heterojunction not only effectively separates the photogenerated charge in composite photocatalysts but also preserves optimal redox capabilities. This study presents the first report of CuInS 2 /CeO 2 (CIS/CeO 2 ) and demonstrates how charge separation within CIS/CeO 2 to enhance photocatalytic hydrogen production through the construction of an S-scheme heterojunction. The UV–visible-driven hydrogen production rate of CIS/CeO 2 is 4.6 and 9.4 times higher than that of CIS and CeO 2 alone, respectively. The improved photocatalytic performance primarily stems from enhanced charge separation promoted by the S-scheme heterojunction. The charge transfer pathway was confirmed as an S-scheme mechanism through a combination of band structure experiments, density functional theory (DFT) calculations on work function, internal electric field, and charge differential density distribution, alongside electron paramagnetic resonance (EPR) experiments. Multiple perspectives were employed to elucidate the reasons behind facilitating efficient charge separation. This research provides valuable insights for advancing photocatalytic performance.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Mengying Xu,Jingyan Zheng,Pier-Luc Tremblay,Xiangyang Jiang,Chun He,Yujie Wang,Muhammad Babur Joya,Tian Zhang
Amid the pursuit of renewable energy, photocatalytic H 2 evolution (PHE) and biosynthetic processes gained attention. Bulk g-C 3 N 4 (CN) was calcined under the atmosphere and various gases (air, CO 2 , N 2 , and Ar) to achieve ultra-thin nanosheets. Using greenhouse gas CO 2 for the calcination (CN–CO 2 ) results in a greater PHE rate than in the atmosphere and air, similar to inert gases N 2 and Ar. Under visible light, CN–CO 2 produced H 2 2.6 times faster than CN. Therefore, CN–CO 2 was chosen to promote polyhydroxybutyrate (PHB) production by Cupriavidus necator H16 in hybrid photosynthetic system. The heterotrophic PHB production was increased to 9.14 g/L, which was 1.9 times higher than without the photocatalyst (4.93 g/L), and 1.1 times more than with CN (8.11 g/L). The autotrophic PHB production was also enhanced by adding CN–CO 2 . In summary, the dual benefits of PHE and biological stimulation were achieved by calcining g-C 3 N 4 in CO 2 .
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ACS Applied Materials & Interfaces
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2017
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IF 7.504
Ping Wang,Minmin Wang,Jie Zhang,Chuanping Li,Xiaolong Xu,Yongdong Jin
Colloidal semiconductor quantum dots (QDs) have recently emerged as a good candidate for photocatalytic hydrogen (H2) evolution in water. A further understanding of the factors that can affect and boost the catalytic activity of the QD-based H2-generating system is of great importance for the future design of such systems for practical use. Here, we report on the fine shell thickness engineering of colloidal CdS/CdSe core/shell QDs and its effect on the photocatalytic H2 production in water. Our results show that, with the proper shell thickness, the H2 photogeneration quantum yield (ΦH2) of CdS/CdSe core/shell QDs could reach 30.9% under the illumination of 420 nm light, which is 49% larger than that of the CdS core. Furthermore, the underlying mechanism has also been tentatively proposed and discussed.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Guojie Liu,Houfang Lu,Kejing Wu,Guoqing Guan,Bin Liang
The interactions between the three major components of lignocellulose significantly affect the thermochemical conversion process and product distribution. Herein, the role of hydrogen bonding and the melting behaviors among the three major components on different H 2 production stages during alkaline thermal treatment (ATT) of lignocellulose are revealed for the first time. The melting behavior of xylan (120 ∼ 210 °C) and the unique hydrogen bonding between cellulose and xylan reinforced by molten xylan (120 ∼ 160 °C) are essentially responsible for the hysteresis of dehydrogenation and formation of active char (160 ∼ 235 °C). Hydrogen bonding gradually disappears during the formation and further reaction of active char. The melting behavior of xylan also hinders the mass transfer of gaseous products at 235 ∼ 350 °C and promotes the methanation reaction of active char. The slight melting behavior of lignin (200 ∼ 250 °C) has minimal effect on the dehydrogenation process, but exacerbates the carbonization reaction of the ATT process, leading to a decrease in H 2 production. Subsequently, the conversion of char is the main reaction above 350 °C and increasing the alkali addition facilitates the efficient conversion of char. Especially, the small discrepancy between the fitted and experimental values of H 2 production from ATT of real lignocellulose provides new insights into establishing a predictive model for H 2 production based on the three major components.
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