INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yining Bao,Qingru Zeng,Shunyan Ning,Wei Zhao,Longfei Wang,Xinpeng Wang,Yuezhou Wei,Deqian Zeng
Developing effective heterojunction photocatalysts that efficiently separate charge carriers and improve light-harvesting capabilities is crucial in addressing energy and environmental issues. Herein, a unique nanocomposite photocatalyst is constructed by attaching CoMn 2 O 4 nanoparticles onto 2D CdS nanosheets for H 2 production and U(VI) reduction. The optimized 2% CoMn 2 O 4 /CdS nanocomposite showcases the highest photocatalytic H 2 production efficiency, 5.8 times higher than CdS nanosheets . Additionally, the U(VI) reduction rate constant of 2% CoMn 2 O 4 /CdS is 0.0192 min −1 , approximately 1.9 folds over the pristine CdS (0.0101 min −1 ). The exceptional photocatalytic performance toward photocatalytic H 2 evolution and U(VI) reduction reactions directly result from the electronic integration between CoMn 2 O 4 /CdS p-n heterojunction, facilitated by the efficient photoexcited charge separation. Feasible photocatalytic mechanisms are proposed through experimental analyses and theoretical calculations. This study provides a straightforward method for designing effective CdS-based heterostructured photocatalysts, contributing to the advancement of solar-to-H 2 conversion and environmental abetment.
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ChemistrySelect
·
2024
·Vol. 9
·期 32
·e202402012
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IF 1.9
KangDi Chen,Siqi Chai,Guoqiang Li,Zeyu Li,Youqian Wang,Heting Li,Liwei Ma,Mai Wei,Guojie Zhang,Ying Wang
Graphical H 2 reduction reduces part of Cu 2+ to Cu + and Ce 4+ to Ce 3+ on the catalyst surface, and Cu and Ce can be stably anchored on the surface of the Cu−Ce/AC catalyst, which effectively improves the dispersion of the Cu component, and then slows down the loss of metal Cu. In this study, we utilized the carbon precursor derived from walnut shells to synthesize a series of Ce-modified Cu-based carbon catalysts (Cu−Ce/AC) via the impregnation method. We investigated the performance and stability of Cu−Ce/AC catalysts for CWAO phenol after H 2 reduction at various temperatures. The Cu−Ce/AC-250 catalyst exhibited its highest performance at 250 °C, achieving complete phenol conversion. Characterization results from techniques including XRD, BET, FTIR, ICP-OES, SEM-EDS, XPS, and H 2 -TPR indicated that the active components of the H 2 -reduced catalysts were more evenly distributed across the catalyst surface, thereby enhancing the availability of reactive sites for phenol oxidation. Simultaneously, under the appropriate temperature, the H 2 atmosphere can reduce a portion of the Cu 2+ on the catalyst surface to Cu + , thereby mitigating the loss of Cu components.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Weidi Qin,Yang Xiao,Chunlei Zhang,Haiyi Gong,Qingsong Zhang,Qingyi Zeng
Photocatalytic hydrogen production and uranium reduction can solve the problems of energy crisis and environmental pollution. Here, bismuth nanocluster loaded on N-doped porous carbon (Bi 0 /NC) with “memory catalysis” effect was prepared through a Bi-MOF precursor pyrolysis strategy for H 2 generation and UO 2 2+ reduction. The photocatalyst achieved an enhanced H 2 production rate of 12.8 mmol g −1 h −1 and an improved UO 2 2+ removal ratio of 95.9 %, which was 3.2 and 1.8 times as pristine carbon material, respectively. Moreover, both the H 2 generation and UO 2 2+ reduction showed a sustained activity under dark condition. Improved activity is ascribed to the optimized electronic property and the enhanced charge separation in Bi 0 /NC, which can be proved by the DFT calculation of projected density of state, Fermi level and charge density difference. This work provides a new strategy to realize the continuous H 2 generation and U(VI) reduction in day and night.
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CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Shuang Li,Haili Lin,Xuemei Jia,Xin Jin,Qianlong Wang,Xinyue Li,Shifu Chen,Jing Cao
Although bimetallic phosphide cocatalysts have attracted considerable interest in photocatalysis research owing to their advantageous thermodynamic characteristics, superstable and efficient cocatalysts have rarely been produced through the modulation of their structure and composition. In this study, a series of bimetallic nickel-iron phosphide (Ni x Fe 2– x P, where 0 < x < 2) cocatalysts with controllable structures and overpotentials were designed by adjusting the atomic ratio of Ni/Fe onto nonmetallic elemental red phosphorus (RP) for the photocatalytic selective oxidation of benzyl alcohol (BA) coupled with hydrogen production. The catalysts exhibited an outstanding photocatalytic activity for benzaldehyde and a high H 2 yield. The RP regulated by bimetallic phosphide cocatalysts (Ni x Fe 2– x P) demonstrated higher photocatalytic oxidation-reduction activity than that regulated by monometallic phosphide cocatalysts (Ni 2 P and Fe 2 P). In particular, the RP regulated by Ni 1.25 Fe 0.75 P exhibited the best photocatalytic performance. In addition, experimental and theoretical calculations further illustrated that Ni 1.25 Fe 0.75 P, with the optimized electronic structure, possessed good electrical conductivity and provided strong adsorption and abundant active sites, thereby accelerating electron migration and lowering the reaction energy barrier of RP. This finding offers valuable insights into the rational design of highly effective cocatalysts aimed at optimizing the photocatalytic activity of composite photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Hang Xu,Lili Jiang,Yan Hu,Jitao Lin,Chao Zhou,Zhijun Zhong,Xiaomin Li,Chuanqiang Yin,Changxin Tang,Lang Zhou
Polyimide (PI) has emerged as a promising material for constructing efficient gas separation membranes due to its excellent stability and gas separation properties. Herein, we report a novel composite membrane structure that utilizes the synergistic effect to achieve efficient H 2 /CO 2 separation by skillfully integrating the advantages of three different functional layers. The support layer consists of a PI fiber membrane loaded with zeolitic imidazolate framework-67 (ZIF-67) using an in-situ growth method, which not only enhances the overall mechanical strength of the membrane, but also provides complex gas transport pathways to improve selectivity. The intermediate layer is made of polydimethylsiloxane (PDMS), which prevents excessive penetration of the selective layer solution into the support layer. The selective layer is a mixed matrix membrane composed of polyetherimide (PEI) as the polymer matrix and zeolitic imidazolate framework-67 (ZIF-67) as the porous filler, which provides critical molecular sieving functionality. Compared to pure polyetherimide (PEI) film, the composite membranes have significantly improved mechanical and gas transport properties, with H 2 permeability of 83.4 Barrer and H 2 /CO 2 selectivity of 5.4. Additionally, the composite membranes exhibit excellent hydrophobicity and thermal stability. Given their outstanding overall performance, the composite membranes developed in this study demonstrate significant potential for CO 2 capture and H 2 recovery applications.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Chunyi Ye,Yang Yang,Shujing Chen,Chunhua Liu,Xiao-Qing Sun,Danni Liu,Jiujun Zhang,Jing-Li Luo,Xian-Zhu Fu
Hydrogen (H 2 ) is a promising green alternative fuel; however, the widespread adoption of H 2 production technologies is limited by high energy consumption and significant carbon emissions. Here, we have developed a bipolar H 2 production electrolyzer that purifies wastewater and produces H 2 with ultra-low energy consumption by combining the formaldehyde 1-electron oxidation reaction (FOR-1) at the anode and the hydrogen evolution reaction (HER) at the cathode. The electroless Cu electrode exhibits high selectivity and activity for the 1-electron pathway of formaldehyde oxidation (i.e., FOR-1), enabling the anodic conversion of formaldehyde into valuable H 2 and formate. This facilitates the treatment of toxic formaldehyde waste while doubling H 2 production efficiency of the electrolyzer. Unlike conventional water electrolysis, the formaldehyde-water electrolyzer demonstrates a cell voltage reduction of 1.49 V at 10 mA/cm 2 . At 100 mA/cm 2 , the energy consumption is reduced to only 25 % of that in conventional systems, even with the use of a nickel foam cathode. Moreover, formaldehyde in wastewater is fully degraded within 50 min, highlighting its practical application potential.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mengli Zhou,Sichan Li,Haojie Tian,Xinyu Liu,Zhimin Wu,Qiying Liu,Jianchun Jiang
Levlinic acid (LA) and its derived γ-valerolactone (GVL) are the two important biomass derived platform molecules, which showed wide application in the fields of fine chemicals, drug and liquid fuel industrials. Considering the coupling of sequential steps for glucose to LA and GVL, selective production of LA and GVL via glucose one-pot conversion in water is an open challenge. Herein, we used metal chlorides as the acidic catalyst for glucose conversion to LA, obtaining the high yield of 77.8 C-mol% over SnCl 4 . Moreover, using the SnCl 4 and Ru/C as the combined catalyst, glucose or cellulose could be converted to GVL with the high yield of 60.1 or 57.9 C-mol% in the case of in situ hydrogenation by formic acid (the by-products during LA formation) decomposition. The formation of LA was responsible for the cooperative effect of BAS (Bronsted acid sites) and LAS (Lewis acid sites) of SnCl 4 for accelerating glucose isomerization, fructose dehydration followed by 5-hydroxymethyl furfural (HMF) rehydration, while the GVL production is relative to the highly efficient formic acid decomposition to H 2 followed by LA hydrogenation to GVL over Ru/C. This study provided an avenue for facile and highly efficient conversion of biomass and the derivatives to LA and GVL using commercial catalysts.
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Surfaces and Interfaces
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2024
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IF 5.7
Guoqiang Zhang,Diandian Shi,Zhiqi Wang,Jianqing Li,Tao He,Jingli Wu,Jinhu Wu
The high-dispersed nano complex ZnO/Co 3 O 4 was first prepared by calcining the ZIF-8@ZIF-67 in Air. Then, the ternary mix-heterojunction ZnIn 2 S 4 /CdIn 2 S 4 /Co 3 O 4 (CdIn 2 S 4 /Z/C) was first in situ constructed by introducing nano complex ZnO/Co 3 O 4 into the CdIn 2 S 4 precursor solution via a solvent thermal reaction. Overall, the CdIn 2 S 4 /Z/C photocatalyst exhibits excellent performance in the photoconversion of CO 2 and H 2 O, which increased by 18.1%∼34.1% for CO, 36.8%∼73.9% for H 2 , and 21.1%∼40.6% for syngas (CO+H 2 ), respectively, compared with CdIn 2 S 4 . The CdIn 2 S 4 /Z/C-40 shows the highest H 2 -evolution rate of 1661.8 μmolg −1 h −1 , which is 87.5% higher than that of CdIn 2 S 4 (886.3 μmolg −1 h −1 ). The CdIn 2 S 4 /Z/C exhibits higher surface S-vacancy concentration, larger specific surface area, stronger light absorption, and photocurrent density than that of CdIn 2 S 4 . The band structure reveals that the ZnIn 2 S 4 /CdIn 2 S 4 /Co 3 O 4 forms a tandem internal electric field at the double heterojunction interface, which is beneficial to improve the migration of photocarrier. This work provides a feasible strategy for constructing synergistic mix-heterojunction photocatalyst for photoconversion of CO 2 and H 2 O.
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ACS Catalysis
·
2024
·
IF 11.3
Zongyi Huang,Pengfei Sun,Huizhen Zhang,Haikun Zhang,Shuhong Zhang,Zhou Chen,Xiaodong Yi,Shunji Xie
The integration of solar-driven H2 evolution with the selective conversion of biomass-derived alcohols into value-added chemicals has gained significant attention for full use of electrons and holes. We develop a dual-functional photocatalyst for highly selective oxidation of the Cα–H bond of benzyl alcohol to C–C coupled products (hydrobenzoin and deoxybenzoin), in cooperation with H2 evolution, using point-to-face interface engineering by decorating CdS quantum dots on Zn2In2S5 nanosheets (CdS QDs/Zn2In2S5 NS). The CdS QDs/Zn2In2S5 NS exhibit a high H2 evolution rate of 13 mmol g–1 h–1 and C–C coupled products formation rate of 10.8 mmol g–1 h–1 with 96.3% selectivity. Benzyl alcohol conversion achieves 91% with an 89% yield of C–C coupled products in gram-scale. The introduction of CdS enhances the interfacial contact, facilitating the efficient spatial separation of photogenerated electron–hole pairs and providing active sites for H2 evolution. In situ characterization and DFT calculation reveal that the carbon-centered radical •CH(OH)C6H5, generated by abstracting the Cα–H bond of benzyl alcohol, is the reactive intermediate in the photocatalytic C–C coupled process.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Zhen Sun,Maonan Ran,Guan Zhang
Solar-driven photocatalytic water splitting for hydrogen production is gaining dramatic interests, however, efficiencies are still not satisfied to make it technically applicable in large scale. Herein, we have observed unconventional high-temperature effects on the change of intrinsic photophysical properties of semiconductors, and demonstrated dual synergistic photothermal effects in promoting hydrogen evolution from water reduction and cellulose pyrolysis at high temperature with metal oxides catalysts. Particularly, Zn/ZnO species deposited TiO 2 (Zn-TiO 2 ) catalyst showcased exceptional thermal-assisted photocatalytic H 2 production from water reduction along with cellulose decomposition at 573 K with quasi apparent quantum efficiency of nearly 100 % under 365±10 nm irradiation and solar to hydrogen (STH) efficiency of 2.72 %. In situ spectroscopic characterizations at 573 K corroborated that the absorption spectrum of Zn-TiO 2 could be extended into the near-infrared region (beyond 1200 nm), and electron-hole pair recombination is curbed and migration of photogenerated charge carriers within the catalyst is remarkably promoted at high temperature. In addition, experimental analysis and molecular dynamics simulations unraveled the synergistic photo-assisted thermal effects for cellulose pyrolysis, and delineated potential pathways for cellulose conversion at high temperature under light irradiation. This work paves the way for efficient utilization of whole solar spectrum for achieving sustainable water splitting and biomass waste utilization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Bin Zhu,Chunlin Chen,Liyuan Huai,Zhenqiang Zhou,Lei Wang,Jian Zhang
Simultaneous production of value-added 2,5-furandicarboxylic acid (FDCA) and H 2 from the integrated 5-hydroxymethylfurfural (HMF) oxidation and hydrogen evolution reaction by electrocatalysis has drawn tremendous attention due to the significantly improved energy efficiency. However, HMF is not thermally and chemically stable enough to often cause heavy degradation, impeding its storage and industrialization. In this work, a more stable furan molecule, 2,5-bis(hydroxymethyl)furan (BHMF), was employed as the reaction substrate into the coupling system for the first time. By means of facile electrodeposition and subsequent oxidative activation, the standing CoOOH nanosheet electrocatalyst was fabricated to realize a complete BHMF conversion with 90.2 % FDCA yield and 100 % current efficiency for H 2 evolution. The reaction path and apparent activation energies were therefore discussed. Scalable properties and electrochemical durability of CoOOH were evaluated in a continuous flow reactor to harvest gram-level solid FDCA, highlighting the prospect of green coupling electrolysis for industrial application.
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Nano-Micro Letters
·
2023
·Vol. 15
·期 1
·1-13
·
IF 26.6
Gao Manyi,Tian Fenyang,Zhang Xin,Chen Zhaoyu,Yang Weiwei,Yu Yongsheng
A hybrid co-catalysts system comprising Au nanoparticles (NPs) and PtSAs with different functions was constructed on the polymeric carbon nitride (PCN) surface by double-solvent method.
For the dual co-catalysts, the Au NPs absorb relatively long-wavelength light to produce plasmonic hot-electrons, and the adjacent Pt single atoms (PtSAs) can trap the plasmonic hot-electrons effectively for H 2 evolution.
The PtSAs–Au 2.5 /PCN exhibits excellent broad-spectrum photocatalytic H 2 evolution activity with the H 2 evolution rate of 8.8 mmol g − 1 h − 1 at 420 nm and 264 μmol g − 1 h − 1 at 550 nm, respectively.
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