JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Shenghong Wang,Changan Zhou,Yongda Cao,Lei Song,Lirong Zheng,Kui Ma,Hairong Yue
Electrochemical water–gas shift (EWGS) reaction is an emerging technology with energy-saving and environmental-friendly advantages to produce high-purity hydrogen form the waste gas containing CO. However, it remains a significant challenge to design superior activity and highly durable EWGS electrocatalysts, particularly with low content of noble metals. Herein, a series of Pt-xCu/Fe 2 O 3 (x = 0, 2, 5) catalysts are synthesized by the complexation precipitation method to construct coupling sites between Pt and CuOx, aiming to optimize the adsorption of CO and the activation of OH – . The obtained 2.5Pt-2Cu/Fe 2 O 3 catalyst presents a unique Pt-O-Cu structure, delivering a much lowest onset potential, high specific activity, and excellent mass activity (1.5 A·mg Pt -1 ) at 0.73 V ( vs. RHE), which is over 15 and 3 times that of commercial Pt/C (20%) and unmodified Pt/Fe 2 O 3 catalyst, respectively. Meanwhile, the in-situ X-ray absorption results demonstrate that the facilitated interaction among the Pt-O-Cu structure promotes the high durability of the 2.5Pt-2Cu/Fe 2 O 3 catalyst and the operability at high potential. More importantly, the moderate binding of CO and moderate activation of OH* are suggested for boosting the reactivity in the CO electro-oxidation reaction. In particular, the fabricated Pt||2.5Pt-2Cu/Fe 2 O 3 , employed in coupling the HER and CO electro-oxide reaction, shows a remarkable hydrogen production of about 98 mmol H2 ·h −1 ·mg Pt −1 at 0.8 V ( vs. RHE). This work also definitely confirms the possibility of the catalyst being applied to produce hydrogen under practical conditions with different concentrations of CO, even being applied in the purification of trace CO in a hydrogen-rich atmosphere.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jing Liu,Bin Zhu,Yang Zhong,Shilin Fan,Liyuan Huai,Hualei Hu,Yong Yang,Jian Zhang,Chunlin Chen
Electrocatalysis using 5-hydroxylmethylfurfural (HMF) as a substrate to produce 2,5-furandicarboxylic (FDCA) is a potentially sustainable and mild route to harvest both value-added chemicals and clean energy hydrogen. However, the poor chemical and thermal stability of HMF has impeded its storage and industrialization. Additionally, the uncontrollability, scalability, and cost of catalyst preparation methods are rarely considered in this field. Herein, we capitalize on the spontaneous and harmful corrosion phenomenon occurring under natural conditions to prepare efficient Co-based catalysts for the electrooxidation 2,5-bis(hydroxymethyl)furan (BHMF) with more stable dihydroxy groups, coupled with hydrogen evolution. The preparation of electrocatalysts through corrosion engineering is a straightforward, cost-effective, highly feasible, and scalable approach, requiring minimal equipment. In the optimal concentration of 200 mM BHMF, an ultrahigh current density of 1981.7 mA cm −2 was achieved at 2.293 V vs. RHE, contributed by both BHMF oxidation and oxygen evolution reaction (OER). Chronoamperometric electrolysis realized efficient FDCA production with 95.4% yield and 96.5% faradaic efficiency (FE) at an ultralow potential of 1.4 V vs. RHE. Since it is etched and grown on the substrate itself, the catalyst prepared by corrosion engineering is very stable and undergoes ten successive chronoamperometric electrolysis without significant structural or performance failure. Moreover, kinetic analyses are investigated to explore the origin of catalytic activity and reaction energy barrier. Finally, to further realize the potential of FDCA and H 2 production in practical application, we innovatively designed a device with a two-electrode electrolyzer and a solar cell in series to drive BHMF electrooxidation with outdoor sunlight. The complete conversion of BHMF only takes 90 min, achieving a 93.5% FDCA yield and nearly theoretical hydrogen evolution.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 15
·4562-4568
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IF 7
Chu-Xuan Liu,Rui Shi,Wangjing Ma,Fulai Liu,Yong Chen
The recycling of plastic waste has attracted increasing attention because of its negative effects on the ecological environment and human health. Photoreforming is emerging as a green and promising approach for upcycling plastic waste into highly valuable chemicals and H2 fuels. Herein, an earth-abundant Ni2P/ZnIn2S4 catalyst prepared by mechanical grinding is reported to selectively photoreform various polyester plastics into high-added-value chemicals coupled with H2 evolution under mild conditions. In particular, polylactic acid (PLA) can be upcycled to pyruvic acid (PA) with high activity (745.9 μmol g−1 h−1) and selectivity (>90%). Moreover, the H2 evolution rate can reach up to 781.3 μmol g−1 h−1 catalyzed by 7.5 wt% Ni2P/ZnIn2S4. This system exhibits excellent photocatalytic performance, benefiting from efficient photogenerated charge carrier separation and transfer between Ni2P and ZnIn2S4. This study provides a viable and promising solution for simultaneously producing high-purity H2 and added-value chemicals from polyester plastic waste, demonstrating its potential for practical recycling applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Xiangbo Feng,Lvwei Sun,Wei Wang,Yuzhen Zhao,Jian-Wen Shi
Photoelectrochemical (PEC) water splitting provides a promising strategy for the production of clean hydrogen fuel. Herein, a new CdS@ZnO core–shell nanorod arrays (NRAs) is successfully constructed by atomic layer deposition (ALD) for H 2 evolution from PEC water splitting. The CdS@ZnO 200 obtained after 200 ALD cycles presents a significantly enhanced PEC H 2 evolution rate of 21.64 μmol·h −1 ·cm −2 , which is about 9.4 times of pristine CdS NRAs (2.31 μmol·h −1 ·cm −2 ). The reasons for the improved PEC H 2 evolution performance can be ascribed to several aspects: firstly, the Z-scheme charge transfer mechanism formed between CdS core and ZnO shell promotes the effective spatial separation of photo-induced electrons and holes; secondly, the close contact between the two semiconductors resulted from ALD process helps to reduce the transfer resistance of charge carriers. In addition, the CdS core is tightly wrapped by ZnO shell, which helps to prevent the photo-corrosion of CdS core. This work provides a new type of photoanode material suitable for PEC H 2 evolution from water splitting, and provides an efficient anti-corrosion method for the use of photocorrosive semiconductor materials.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Jingwei Li,Zhengyi Huang,Cong Wang,Lei Tian,Xiaoqing Yang,Rongfu Zhou,Mohamed Nawfal Ghazzal,Zhao-Qing Liu
Refining carrier transfer in bandgap-broken heterojunctions, which consist of two semiconductors with broken bandgaps, is crucial yet highly challenging for photocatalysis. Herein, we incorporated amorphous carbons (AC) into the bandgap-broken V 2 O 5 /GdCrO 3 heterojunctions, inducing a linkage effect to facilitate photoexcited carrier transfer. The created V-O-C and Cr-O-C bonds in V 2 O 5 -AC-GdCrO 3 interfaces show almost identical orbital energies to overcome the broken-gap energy barriers at interfaces. The holes at GdCrO 3 ’s valence band and electrons at V 2 O 5 ’s conduction band tent to migrating toward the carbon ring of amorphous carbon via Cr-O-C and V-O-C bonds, thereby enhancing carrier separation of bandgap-broken V 2 O 5 /AC/GdCrO 3 heterojunction. By controlling the relative amount of metal-O-C bonds in the interface, the modulation of charge transfer kinetics was also achieved on V 2 O 5 /AC/GdCrO 3 , resulting in ∼7 times higher of H 2 generation than V 2 O 5 /GdCrO 3 . The concept could be expanded to the other carbon allotropes, including graphene, carbon nanotube, and graphdiyne conjugated structures, demonstrating a universal strategy in reaching optimal charge transfer of broken-bandgap heterojunctions for photocatalytic H 2 production.
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Catalysts
·
2022
·Vol. 12
·期 9
·1043
·
IF 4.501
Shuang Tang,Yang-Sen Xu,Wei-De Zhang
Molecular skeleton modification has become a recognized method that can effectively improve the photocatalytic performance of g-C3N4because it not only effectively promotes charge separation, but also tunes the conjugated system of g-C3N4to make it more conducive to photocatalytic reaction. Herein, thiophene-amide embedded g-C3N4(TA-CN-x) was successfully prepared by simple one-step thermal polycondensation using urea as a precursor and ethyl-2-amino-4-phenylthiophene-3-carboxylate (EAPC) as an additive. After embedding with thiophene-amide, the induction and delocalization effects are formed in TA-CN-x, which significantly improves the migration efficiency of photogenerated charge carriers. Meanwhile, the conjugate structure is changed due to structural modification, resulting in significant enhancement of visible light absorption compared to the pure g-C3N4(CN). Specifically, the optimized photocatalytic H2evolution rate of TA-CN-2 reaches 245.4 μmol·h−1, which is 8.4 times that of CN (with Pt nanoparticles as a co-catalyst), and the apparent quantum efficiency (AQY) at 450 nm is 13.6%. This work opens up a new modification process for fully tapping the photocatalytic hydrogen absorption potential of g-C3N4-based materials.Keywords:photocatalysts;g-C3N4;thiophene-amide;embedding;induction effect;delocalization effect;hydrogen evolution
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Chang-An Zhou,Shenghong Wang,Kui Ma,Lei Song,Lirong Zheng,Hairong Yue
The sluggish kinetics and high overpotential of oxygen evolution reaction (OER) at anode hinders water splitting large-scale application. Recently, an anode alternative strategy exhibits promising prospect of application to improve reaction kinetics and decrease overpotential. Here, single dispersed Ru-anchored porous Pt 3 Ni alloy (Ru 1 -Pt 3 Ni/NiF) were successfully synthesized via spontaneous galvanic reduction, over which highly selective electrooxidation of ethanol into acetate was realized. DFT calculations show that Ru modification introduced abundant active oxygen species (OH*), which not only enhanced the oxidation activity of ethanol, but also increased the selectivity for C2 oxidation pathway. Then a Ru 1 -Pt 3 Ni/NiF||Pt 3 Ni/NiF ethanol oxidation membrane-free cell was built to couple the ethanol electrooxidation with H 2 evolution, where the Faraday efficiency of H 2 production reaches 94% and the power consumption is 19.24 kWh kg H2 −1 . This work provides a cost-competitive and energy-saving strategy for high-purity H 2 generation, opening new opportunities for electric energy utilization from renewable sources.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 44
·21078-21084
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IF 3.925
Xing-Liang Yin,Lei-Lei Li,Yan-Lan Wang
An efficient and stable CdS@MoS2 core@shell heterostructure was prepared by using a facile solvothermal approach. The MoS2@CdS heterostructure reveals efficient charge separation, giving rise to excellent performance on H2 generation from photocatalytic lactic acid decomposition. Thanks to the MoS2 shell protection, CdS corrosion was significantly prohibited, thus resulting in the long-term photocatalytic stability of the CdS@MoS2 heterostructure. The corresponding charge transfer properties and catalytic mechanism have been analyzed and discussed in detail. The present study provides a novel insight into the design of high performance and cost-effective photocatalysts.
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CHINESE JOURNAL OF CATALYSIS
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2022
·
IF 12.92
Jiang Zhang,Zijian Wang,Mugeng Chen,Yifeng Zhu,Yongmei Liu,Heyong He,Yong Cao,Xinhe Bao
Deoxygenative upgrading of 5-hydromethylfurfural (HMF) into valuable chemicals has attracted intensive research interest in recent years, with product selectivity control remaining an important topic. Herein, TiO 2 supported gold catalysts coated with a thin N-doped porous carbon (NPC) layer were developed via a polydopamine-coating-carbonization strategy and utilized for pathway-specific conversion of HMF into 5-methylfurfural (5-MF) with the use of renewable formic acid (FA) as the deoxygenation reagent. The as-fabricated Au/TiO 2 @NPC exhibited excellent catalytic performance with a high yield of 5-MF (>95%). The catalytic behavior of Au@NPC-based catalysts was shown to be correlated with the suitable combination of highly dispersed Au nanoparticles and favorable interfacial interactions in the Au@NPC core-shell hetero-nanoarchitectures, thereby facilitating the preferential esterification of HMF with FA and suppressing unproductive FA dehydrogenation , which promoted the selective formylation/decarboxylation of hydroxy-methyl group in HMF in a pathway-specific manner. The present NPC/metal interfacial engineering strategy may provide a potential guide for the rational design of advanced catalysts for a wide variety of heterogeneous catalysis processes in terms of the conversion of biomass source.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yu Wang,Yunlei Shi,Dazhen Xiong,Zhiyong Li,Huiyong Wang,Xiaopeng Xuan,Jianji Wang
Ammonia (NH 3 ) is produced from nitrogen (N 2 ) and hydrogen (H 2 ) by the Harber-Bosch process at high pressure and high temperature. Due to the reversibility and low conversion efficiency of the reaction, the product contains a large amount of raw gas, which seriously affects the production efficiency of ammonia. Therefore, it is essential to exploit high-performance adsorbents for separating NH 3 from NH 3 /N 2 /H 2 mixtures. Herein, we designed and synthesized a kind of metal–organic framework (MOF) composites by anchoring metal chloride (NiCl 2 , CoCl 2 , or SnCl 2 ) on the bipyridinium groups in the MOF-253(Al) pores. It is found that the optimal composite shows an NH 3 uptake capacity of 18.0 mmol/g at 25.0 °C and 1.0 bar, which is 3.33 times that of the pristine MOF-253(Al), and the composite exhibits a much faster adsorption kinetics of NH 3 than the pristine MOF-253(Al). Significantly, the excellent NH 3 uptake capacity at low pressure allows selective trapping of NH 3 from NH 3 /N 2 /H 2 at 25.0 °C with the selectivity coefficients of 5708 to N 2 and 2320 to H 2 . Spectral measurements reveal that the synergistic action of NH 3 coordination to the metal in the MOF and the hydrogen bonding of NH 3 with both O atoms of the carboxyl groups and Cl − of the guest molecules account for such an excellent capture and selectivity. In general, the strategy developed here is simple and effective for improving the selectivity of NH 3 separation, which opens a new way for the design of high-performance solid adsorbents.
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Nanoscale
·
2023
·Vol. 15
·期 37
·15238-15248
·
IF 6.7
Nan Zhang,Gang Li,Zhichao Yu,Zhenguo Tang,Xiaoyan Liu,Congwei Wang,Kaiying Wang
Heterostructure interfacial engineering between photocatalyst and co-catalyst to obtain an optimized electronic structure is a promising approach to improving their performance in the photocatalytic hydrogen evolution reaction (HER). In this work, two-dimensional nanopetal-like ZnIn2S4 (ZIS) with an adequately exposed active (110) edge facet-decorated Ni cluster heterostructure was prepared via chemical bath deposition, followed by photodeposition. In the catalyst preparation, the ZIS microstructure was modulated to sufficiently expose the active sites of the (110) edge for the HER, on which spontaneous interfacial engineering with an additional Ni cluster co-catalyst would be triggered via photodeposition in situ. The hydrogen production rate of the composite photocatalyst was excellent, at up to 26.80 mmol g−1 h−1 under simulated sunlight, which was 15.4 times greater than that of pristine ZIS. The optimized photocatalyst achieved a state-of-the-art apparent quantum yield of 61.68% at a single wavelength of 420 nm. Combined with systematic experimental characterization and density functional theory calculation, it was demonstrated that the separation and migration of charge carriers were significantly enhanced via the Ni cluster-induced interfacial electron redistribution, which contributed to the near-zero Gibbs free energy barrier and favored intermediate (*H) adsorption and desorption behavior, resulting in the superior photocatalytic performance. In summary, this work enables tuning of the interfacial electronic properties via spontaneous photodeposition of metallic cluster co-catalyst on the edge active sites, through which the separation of photogenerated charge carriers and surface redox reactions can be synergistically facilitated.
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PubMed
高影响因子
Nano Energy
·
2021
·
IF 17.881
Xue Li,Jundie Hu,Tingyu Yang,Xiaogang Yang,Jiafu Qu,Chang Ming Li
Effectively utilize photogenerated holes (h + ) of catalysts while blocking rapid recombination of photoinduced carriers are the two critical challenges for solar-to-hydrogen (STH) conversion. Here, an exquisite 2D/2D LaVO 4 /g-C 3 N 4 (LaVO 4 /CN) heterostructure is delicately designed and fabricated for efficient photocatalytic H 2 -evolution while producing high value-added furfural simultaneously. The abundant biomass furfuryl alcohol (FFA) is employed to substitute the traditional h + sacrificial agents such as triethanolamine (TEOA) for the oxidation half reaction, which is very meaningful to balance the H 2 -evolution half reaction. The LaVO 4 /CN heterojunction enables 3-time increased H 2 -evolution and a high furfural-production rate (0.95 mmol g −1 h −1 ) than that of pristine graphite carbon nitride (g-C 3 N 4 , labeled as CN), and with a 22.16% H 2 -evolution apparent quantum efficiency (AQE) irradiated at 400 nm. This work provides an exquisite catalyst and a new strategy for efficient photocatalytic H 2 -evolution coupled with production of high valuable chemicals.
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