SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Ning Wei,Sufeng Zhang,Xue Yao,Yao Feng,Valentin Nica,Jinfan Yang,Qiusheng Zhou
Biomass electrocatalytic-conversion coupled with hydrogen generation exhibits low energy consumption, efficient hydrogen production and green syntheses of value-added chemicals. However, constructing electrocatalysts with precise electronic modulation and structures for efficient biomass electrocatalytic conversion coupled hydrogen production remains challenging. Herein, a bacterial cellulose substrate was combined in situ with a Mn-doped NiFe Prussian blue analogue (PBA) precursor, and one-step carbonization-phosphorylation was developed for the preparation of Mn-doped nickel iron phosphate (MNFP) embedded in a P, N codoped carbon (PNC) substrate grown directly on P-doped carbonized bacterial cellulose (MNFP-PNC/PCBC). Benefiting from the three-dimensional network structure of P-doped carbonized bacterial cellulose (PCBC) and atomic doping, MNFP-PNC/PCBC exhibited an optimized electronic structure, abundant active sites and excellent electrical conductivity. Therefore, the voltages required with hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and glucose electrocatalytic-conversion (GCR) to drive a current density of 50 mA cm −2 were 0.214, 1.5, and 1.34 V, respectively. Moreover, the required cell voltage of the novel electrolyser containing MNFP-PNC/PCBC as electrodes can be further reduced to 1.55 V at 50 mA cm −2 compared to overall water splitting, resulting in more than 8-time improvement in hydrogen production efficiency and production of value-added formate. This work provides a unique approach for electrocatalytic-conversion of biomass coupled with electrocatalytic hydrogen generation.
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RSC Advances
·
2020
·Vol. 10
·期 33
·19169-19177
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IF 3.119
Biao Zhou,Bo Yang,Muhammad Waqas,Ke Xiao,Caizhen Zhu,Ling Wu
Constructing a 0D/3D p–n heterojunction is a feasible strategy for accelerating photo-induced charge separation and promoting photocatalytic H2 production. In this study, a 0D/3D MoS2/g-C3N4 (0D/3D-MCN) photocatalyst with a p–n heterojunction was prepared via a facile light-assisted deposition procedure, and the 3D spongy-like g-C3N4 (3D-CN) was synthesized through simple thermolysis of NH4Cl and melamine mixture. For comparison, 2D-MoS2 nanosheets were also embedded in 3D-CN by a solution impregnation method to synthesize a 2D/3D-MCN photocatalyst. As a result, the as-prepared 0D/3D-MCN-3.5% composite containing 3.5 wt% 0D-MoS2 QDs exhibited the highest photocatalytic H2 evolution rate of 817.1 μmol h−1 g−1, which was 1.9 and 19.4 times higher than that of 2D/3D-MCN-5% (containing 5 wt% 2D-MoS2 nanosheets) and 3D-CN, respectively. The results of XPS and electrochemical tests confirmed that a p–n heterojunction was formed in the 0D/3D-MCN-3.5% composite, which could accelerate the electron and hole movement in the opposite direction and retard their recombination; however, it was not found in 2D/3D-MCN-5%. This study revealed the relationship among the morphologies of MoS2 using g-C3N4 as a substrate, the formation of a p–n heterojunction, and the H2 evolution activity; and provided further insights into fabricating a 3D g-C3N4-based photocatalyst with a p–n heterojunction for photocatalytic H2 evolution.
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ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Yanwei Sun,Chunshan Song,Xinwen Guo,Yi Liu
Preferred orientation has proven to exert a significant impact on the gas separation performance of metal–organic framework membranes. Nevertheless, realizing three-dimensional orientation control remains a challenging issue. In this study, well-intergrown NH2-UiO-66 membranes with both (111) out-of-plane and regional in-plane orientations were prepared by combining oriented deposition of seeds and solvothermal epitaxial growth. Dynamic air–liquid interface-assisted self-assembly method was employed to organize uniform octahedral-shaped NH2-UiO-66 seeds into closely packed monolayers with (111) out-of-plane and regional in-plane orientations, whereas the use of ZrS2 as the zirconium precursor during the solvothermal epitaxial growth was found indispensible for sealing the intercrystalline gaps while preserving the preferred orientation inherited from seed layers. In addition, compared with solvothermal heating, employing microwave heating led to poor intergrowth between neighboring NH2-UiO-66 crystals because of a lower dielectric loss factor of the reaction medium. Gas permeation results indicated that the prepared NH2-UiO-66 membranes exhibited H2/CO2 selectivity up to 5.5 times higher than their counterparts with random and/or mere out-of-plane orientations as well as H2 permeability 14.5 times higher than NH2-MIL-125(Ti) membranes with mere out-of-plane orientation under similar operating conditions.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2015
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IF 7.435
Zhifeng Jiang,Deli Jiang,Zaoxue Yan,Dong Liu,Kun Qian,Jimin Xie
Novel TiO 2 –In 2 O 3 @g–C 3 N 4 hybrid system was synthesized by a facile solvothermal method. The photocatalytic activity of the TiO 2 –In 2 O 3 @g–C 3 N 4 hybrid material was evaluated via degradation of RhB and hydrogen-production. It could be found that TiO 2 –In 2 O 3 @g–C 3 N 4 ternary composites exhibit the highest RhB degradation rate, which was 6.6 times than that of pure g–C 3 N 4 . As expected, the H 2 -generation rate of the as-prepared ternary materials was found to increase by 48 times than that of pure g–C 3 N 4 . The enhanced activities were mainly attributed to the interfacial transfer of photogenerated electrons and holes among TiO 2 , In 2 O 3 and g–C 3 N 4 , leading to the effective charge separation on these semiconductors, which were evidenced by photoluminescence spectroscopy, electrochemical impedance spectroscopy and photocurrent analysis. The photocatalytic mechanism and photostability of the ternary hybrid materials were also proposed. This work may provide a stepping stone towards the design and practical application of multifunctional hybrids photocatalysts in the photocatalytic degradation of pollutions and hydrogen generation.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Shuang Luo,Chenghua Zhang,Xingyan Liu,Yue Li,Lei Tang,Min Fu,Song Wang,Jie Wu,Mengmeng Xu,Xiaoping Wang,Youzhou He
A novel protonated NH 2 -MIL-125 was fabricated to introduce the moiety with charge and ample hydrogen (–NH 3 + Cl - group) into NH 2 -MIL-125 using HCl vapor obtained by natural volatilization of hydrochloric acid as a protonating reagent, which could exhibit excellent photocatalytic activity in both hydrogen production and NO purification under visible light irradiation. The hydrogen production and NO purification rate of the best protonated NH 2 -MIL-125 were 6762.80 μmol g −1 and 49.17%, respectively, which were 20.53 and 1.84 times as that of the original NH 2 -MIL-125. A series of characterizations, such as Mott-Schottky, PL, FT-IR and in situ DRIFTS , etc. were used to characterize the photoelectrochemical properties of the optimal catalyst, which demonstrated the protonation effect can not only enhance the electron migration rate, but also effectively accelerate photo-generated electron-hole pairs separation in the photocatalytic reaction process. This research believed that using HCl vapor as a facile protonation reagent to introduce the moiety with charge and ample hydrogen (–NH 3 + Cl - ) was a very effective method to decorate MOFs for hydrogen evolution and NO removal.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
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IF 6.371
Xiaohui Ma,Wenjun Li,Chaojun Ren,Hongda Li,Xinyang Li,Mei Dong,Ying Gao,Tianyu Wang,Hualei Zhou,Yanyan Li
Herein, we report the synthesis of ZnIn 2 S 4 nanoparticles on bulk WC by a facile hydrothermal process to construct novel and highly efficient noble metal-free Schottky junction heterojunction photocatalysts. Morphology characterization revealed that the ZnIn 2 S 4 nanoparticles were deposited on the surface of the WC. Meanwhile, the combination of the ZnIn 2 S 4 and the metal-like WC formed the Schottky energy barrier, which greatly promoted the migration and separation of photo-generated carriers. Especially, the optimal ZnIn 2 S 4 /WC photocatalysts have a lower overpotential for hydrogen evolution (−0.35 V) than pristine ZnIn 2 S 4 (−0.49 V). The hydrogen production ability of the optimal ZnIn 2 S 4 /WC photocatalyst (2400.3 μmol·h −1 ·g −1 ) was approximately 9.2 times higher than that of ZnIn 2 S 4 -1% Pt (260.1 μmol·h −1 ·g −1 ). Photocatalytic experiments demonstrated that metal-like WC plays an important role in replacing precious metal to increase the active site of ZnIn 2 S 4 . Moreover, a feasible Schottky junction reaction mechanism of intensive photocatalytic activity was discussed. This study proves that it is a very fascinating strategy to combine the advantages of ZnIn 2 S 4 and metal-like to construct Schottky heterojunction for photocatalytic hydrogen production.
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Journal of Inorganic and Organometallic Polymers and Materials
·
2020
·Vol. 30
·期 11
·4350-4360
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IF 1.941
Zhang Zhihua,Peng Xinke,Zhang Zhongping,Xiao Weiming,Deng Shengjun,Mao Xuejin,Hong Sanguo,Chen Chao,Zhang Ning
Metal–organic framework (MOF) supported nanocatalysts are attracting great attentions in heterogeneous catalysis. However, they are still less explored and poorly understood in catalyzing solid–gas reactions. In current work, two MOF supported Pt nanocatalysts were prepared by immersion method coupled with the most commonly used NaBH 4 (Pt/UiO-66-NaBH 4 ) and H 2 (Pt/UiO-66-H 2 ) reduction, and their catalytic CO oxidation performances were investigated. NaBH 4 and H 2 reduction both provide highly dispersed Pt/UiO-66 nanocatalysts, and the two prepared catalysts display excellent CO oxidation activities. Moreover, CO oxidation durability tests reveal that Pt/UiO-66-NaBH 4 shows superior durability and structure stability, which are much better than those of Pt/UiO-66-H 2 . The high structure stability of Pt/UiO-66-NaBH 4 also endows it with good H 2 O and CO 2 tolerance. This work attempts to elucidate the influence of reduction methods on the structures and catalytic CO oxidation performances of Pt/UiO-66 catalysts by employing XRD, TEM, N 2 -sorption, XPS and in situ DRIFTS techniques. Furthermore, the mechanism of CO oxidation was studied by in situ DRIFTS, and the result reveals that the CO oxidation on the two catalysts follows different mechanism.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Zexiao Zheng,Irene M.C. Lo
Pharmaceuticals and personal care products (PPCPs) and Escherichia coli ( E. coli ) are ubiquitous in sewage posing adverse effects on both ecosystems and human health. Herein, we propose a multifunctional photoelectrochemical (PEC) system to simultaneously degrade PPCPs, disinfect E. coli , and produce H 2 . To this end, an optimized MoS 2 @BL-BiVO 4 photoanode with reduced bulk and surface charge recombination was synthesized, exhibiting a photocurrent density of 2.21 mA/cm 2 at 1.0 V vs. Ag/AgCl in actual sewage, 8.1 times that of P-BiVO 4 . The MoS 2 @BL-BiVO 4 photoanode achieved complete degradation of 2 ppm benzophenone-3 and inactivation of E. coli in sewage with 89.32 μmol H 2 evolution at 1.0 V vs. Ag/AgCl in 30 min. Chloride ions in the sewage played a critical role in the PEC system: they were activated to become chloride-based radicals ( Cl, ClO) for sewage treatment and worked as hole scavengers to increase H 2 evolution. Natural organic matters in the sewage played a dominant role in impeding the PEC reactions because they can quench the reactive species and were adsorbed onto the photoanode’s surface to block charge separation. The PEC system shows good efficiency when degrading various PPCPs, and excellent reusability and stability, giving it great practicality.
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WATER RESEARCH
·
2025
·
IF 12.4
Delong Yu,Guoquan Zhang,Xiaoli Lv,Xiaochen Xu,Fenglin Yang
Achieving efficient NH 4 + -N degradation into harmless N 2 and simultaneous harvesting hydrogen energy is of great significance for protecting aquatic ecosystems and alleviating energy shortages. Herein, a photoelectrochemical-chlorine (PEC-Cl) system was developed aiming to selective converting ammonia to N 2 with simultaneous H 2 evolution in a wide pH range of 3–13. The Pt decorated black TiO 2 nanotube arrays (Pt/BTNAs) with sufficient oxygen vacancies defects and the enhanced PEC properties were synthesized as the bifunctional electrode. The parameters optimization illustrated high N 2 selectivity (88 %) and H 2 yield rate (67.5 μmol cm -2 h -1 ) at pH 9. The ClO • derived from the cross reactions between active chlorine and HO • plays a predominant role in oxidizing ammonia. More importantly, the Gibbs free energy calculation indicated that Pt decorating can also significantly promote the direct electrochemical ammonia oxidation reaction (AOR) on Pt/BTNAs anode. Under alkaline conditions (pH 9–13), the efficient removal and conversion of ammonia into N 2 in the PEC-Cl system was achieved primarily through the direct anodic AOR, with N 2 selectivity (89 %-93 %) and H 2 yield rate (60.9–68.6 μmol cm -2 h -1 ) comparable to those of the ClO • -mediated indirect AOR. This study presents a flexible method for treating high and medium-concentration NH 4 + -N and simultaneously producing H 2 through the synergistic PEC-Cl and direct electrochemical AOR processes, across a wide pH range.
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 8
·2482-2489
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IF 6.177
Nan Sun,Yong Zhang,Xinru Li,Yuhan Jing,Zhengdong Zhang,Yu Gao,Jianqi Liu,Honglin Tan,Xiaoming Cai,Jinming Cai
Copper-based photocatalysts have attracted considerable attention because of their great prospects in photochemical conversions. However, there are still challenges faced during the preparation of copper-based photocatalysts with have high catalytic efficiency and high stability. In this study, polyaniline (PANI) was doped in an ultra-thin graphitized polyacrylonitrile (g-PAN) layer (denoted as CI), and Cu nanoparticles (NPs) were wrapped in the CI layer encapsulated on SrTiO3 (STO), which is designed as an efficient and low-cost photocatalyst for photocatalytic hydrogen production under visible light irradiation. Benefiting from the unique CI layer structure, the optimized Cu@CI/STO photocatalytic hydrogen evolution rate obtained was 371 μmol g−1 h−1, which is higher than the hydrogen evolution rate of Cu@g-PAN/STO (265.25 μmol g−1 h−1). Moreover, the CI layer demonstrated a quasi-cocatalyst effect. The ultra-thin CI layer not only protects the Cu NPs from oxidation but also promotes charge separation, which distinctly boosts H2 evolution, as indicated by the photoluminescence emission spectra, EIS Nyquist diagram and Mott–Schottky diagram. In addition, the degradation rate of Cu@CI/STO is approximately 4-fold higher than that of Cu/STO in the photocatalytic degradation of 4-nitrophenol under visible light. This study delivers a new method to protect Cu NPs and demonstrates the prospect for the rational design of copper-based photocatalysts with high stability and efficiency.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Enming Ping,Xiaoxiao Chen,Yunshan Zhou,Lijuan Zhang,Lingyun Kong,Nan Chen
In this work, CAU-10-H@γ-AlOOH is prepared, and then UTSA-16 is loaded on CAU-10-H@γ-AlOOH to obtain UTSA-16@CAU-10-H@γ-AlOOH. Using the as-prepared composites as stationary materials by cryogenic gas chromatography at 77 K, while CAU-10-H@γ-AlOOH achieves the complete separation of ortho-H2 (o-H2) and D2 with a resolution R of 1.66 and a separation time t of 9.52 min, UTSA-16@CAU-10-H@γ-AlOOH achieves higher efficiency separation of hydrogen isotopes in a shorter separation time (4.56 min) with R = 1.7. Molecular simulation results show that CAU-10-H has both chemical affinity quantum sieving and kinetic sieving effects for H2/D2 at 77 K, and UTSA-16 can only exert the kinetic sieving effect. UTSA-16’s load on CAU-10-H@γ-AlOOH weakens the adsorption of hydrogen isotopes, and the presence of Co2+ in UTSA-16 promotes the conversion of para-H2 to ortho-H2. In gas chromatography, H2 was preferentially desorbed from the system due to strong D2 adsorption caused by the chemical affinity quantum sieving effect and faster H2 diffusion caused by the kinetic sieving effect. These additive effects achieved efficient hydrogen isotope separation at 77 K.
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International Journal of Greenhouse Gas Control
·
2024
·
IF 4.6
Kang Shunji,Shen Zhi,Liu Baiqiang,Yi Qun,Ma Jun,Song Hao,Shen Xizhou
The petrochemical industry has a significant demand for high-purity hydrogen. It primarily obtained from the H 2 purification unit by using pressure swing adsorption (PSA) technology to recover H 2 from medium-temperature shifting gas (MTSG). The the coupled wet CO 2 separation-PSA process was introduced in this work, aiming to capture CO 2 from MTSG while simultaneously increasing the H 2 recovery rate. To enhance the desorption pressure of CO 2 separation unit in the coupled process to facilitate the storage or utilization of the captured CO 2 , firstly, a rigorous thermodynamic study was carried out to provide a theoretical basis for the development of an improved CO 2 solvent. Subsequently, a pilot-scale test was executed to validate the theoretical findings. Finally, the patented coupled process was implemented at an industrial scale for the first time. The results showed that the capacity of PSA unit for H 2 purification increased from 6800 to 12,000 tons per year and the H 2 recovery rate increased from 84.6 % to 93.6 %; the CO 2 desorption pressure increased from about 0.03 MPa (traditional Benfield process) to 0.15 MPa, which reduced the energy consumption of CO 2 compression, and the total average annual economic benefits increased by US $ 15.55 million.
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