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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

Enhanced H2 sensing performance of Pd-modified ZnO nanorods under visible light excitation

Yan Wang,Yihui Wang,Xueya Sun,Mengwei Li,Mingxin Tang,Jianliang Cao,Cong Qin

High-performance room-temperature hydrogen (H 2 ) sensors are the optimal choice for practical applications. Light excitation , especially visible light, is safer and requires less power compared to ultraviolet (UV) light. This makes it an effective method for achieving room temperature operation. In this study, different mass ratios of Pd-modified ZnO nanorods were synthesized using a combination of hydrothermal and impregnation methods, and their sensing performance to H 2 under visible light excitation was investigated. Material characterization results demonstrated that the localized surface plasmon resonance (LSPR) effect of Pd broadened the absorption in the visible light region, increasing the generation of high-energy hot electrons . Notably, the 2.5 wt% Pd/ZnO exhibited excellent sensing performance towards 5000 ppm H 2 at room temperature under visible light excitation, with a high response value of 5906.78. The LSPR effect and the catalytic activity of Pd nanoparticles significantly enhance the sensing performance of H 2 . Based on our current knowledge, there have been no explicit reports on the detection of H 2 using visible light excitation with Pd/ZnO, thus highlighting a new direction for the study of room temperature H 2 sensors.

CAS / MDL: 7647-10-1
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CHEMICAL ENGINEERING SCIENCE · 2023 · IF 4.7

Dual-module integration of large-area tubular 2D MXene membranes for H2 purification

Mide Luo,Yali Zhao,Yanying Wei,Haihui Wang

Construction of large-area two-dimensional (2D) nanosheet membranes for gas separation, particularly tubular membranes, is extremely challenging. Here, electrophoretic deposition technology was employed to construct large-area tubular 2D MXene membranes for H 2 /CO 2 gas separation, where the membrane with a single tube area of 25 cm 2 could be successfully manufactured in approximately 5 min under optimal process conditions. The membrane exhibited good H 2 /CO 2 separation performance with H 2 /CO 2 selectivity of 53.0 and hydrogen permeance of 133.8 GPU, exceeding the 2008 Robeson upper bound, and showed excellent stability in long-term test with water vapor evaluations for more than 350 h. Additionally, some engineering issues and operation parameters concerning the separation performance of H 2 /CO 2 in single-module and dual-module separators have been thoroughly investigated and analyzed. This work has taken an important step toward the industrialization of 2D MXene membranes and also provided significant guidance to other 2D material-based membranes in approaching practical applications.

CAS / MDL: 7789-24-4
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

H2S cracking to produce H2 through microwave discharge catalysis of graphitized petroleum coke

Zhiyang Zhao,Dongqiang Cai,Juan Liu,Guifu Zou,Qiang Zhang,Zhanlong Song,Cuiping Wang,Longzhi Li

Direct cracking of hydrogen sulfide (H 2 S) can be used to obtain high purity hydrogen (H 2 ), thus avoiding the waste of hydrogen resources by the traditional Krauss process. Microwave-induced discharge of spherical graphitization petroleum coke (PC) was proposed to solve the problem of low efficiency and high energy consumption of H 2 S cracking. The PC was prepared by microwave-assisted desulfurization and metal (Fe, Co) catalytic graphitization to obtain better discharge effect. Subsequently, the graphitized PC was applied to induce microwave discharge, and the effects of graphitization parameters on the discharge performance were discussed. Lastly, the attention was concentrated on multi-effects catalytic decoupling and cracking kinetic properties of microwave-induced discharge for H 2 S cracking. PC with Fe 1 /Co 2 loading exhibited greater graphitization degree ( I D / I G  = 1.027) (30.7 % than petroleum coke), brought stronger discharge intensity (initial and ending intensity at 4.08 V and 2.73 V in one-hour), and better discharge stability (67 % after one-hour) compared to PC raw coke. H 2 S cracking through microwave discharge catalysis exhibited a favorable catalytic effect, obtained a complete conversion at the initial stage and remained 95.58 % after one-hour, with H 2 yield of 98.1 %. With Fe 1 /Co 2 loading, H 2 S cracking had the least activated energy, 14.96 kJ/mol, which was the multi-effects of microwave discharge catalysis, thermal-catalysis and Co-catalysis. It was further calculated that discharge-catalysis dominated in H 2 S cracking, with the highest contribution, followed by Co-catalysis, and thermal-catalysis had the lowest contribution.

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ORGANOMETALLICS · 2023 · IF 2.8

Synthesis of Carboxylic Acids via Reaction of Ketones/Aldehydes with CO2 and H2

Yanru Zhang,Jingjing Zhang,Ying Wang,Yang Li,Jun He,Yanyan Wang,Longbo Zhang,Zhenpeng Wang,Qingli Qian,Buxing Han

Synthesis of basic C2+ chemicals using CO2 and H2 is very promising. Herein, we present a protocol for the synthesis of different carboxylic acids by the reaction of ketones or aldehydes with CO2 and H2. The catalytic system consisted of the IrCl3 catalyst, LiI promoter, and acetic acid solvent. The yield can reach 52.9% based on the cyclohexanone substrate which can be derived from biomass. Various Cn ketones and aldehydes could be used as a substrate in the reaction, where the corresponding Cn+1 carboxylic acids were obtained. According to the mechanistic study, the reaction involved substrate conversion, reverse water–gas shift (RWGS) reaction, and carbonylation. This strategy provides an optional way of carboxylic acid production and CO2 utilization.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Hybrid acid/alkali electrolysis toward industrial-scale H2 generation and sulfite oxidation conversion

Luocai Yi,Ping Shao,Hao Li,Mengtian Zhang,Xi Liu,Peng Wang,Zhenhai Wen

Co 2 P has been widely applied in a variety of applications yet still faces challenges in implementing hypotoxic and large-scale synthesis. We here report a scalable synthetic route to produce tussock-like nanostructured Co 2 P (t-Nano Co 2 P), which exhibits high-performance electrocatalytic properties toward acidic hydrogen evolution reaction (HER). Such t-Nano Co 2 P can evolve to CoOOH nanoplates that show excellent electrocatalytic activity for sulfite oxidation reaction (SOR) in alkaline solution. The findings encourage us to construct a hybrid acid/alkali electrolyzer with t-Nano Co 2 P and its CoOOH derivative as catalysts of acidic cathode for HER and alkaline anode for SOR, respectively, which performs excellently with capability of synchronous generation of H 2 and sulfate in an industrial-level rate at a relatively low applied voltage. The proof-of-concept electrolyzer, by virtue of the viability of scalable synthesis and high-production yield, holds great promise for co-production of H 2 and sulfate in an energy-effective and environmentally-friendly manner.

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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Construction of electron donor–acceptor Z-scheme heterojunction for boosting photocatalytic H2 production

Xinlei Zhang,Xuehua Wang,Guicun Li,Lei Wang,Jianfeng Huang,Alan Meng,Zhenjiang Li

Enhancing the solar energy conversion of metal-free graphitic carbon nitride (g-C 3 N 4 ) based photocatalyst remains a great challenge. Herein, a novel Z-scheme heterojunction photocatalyst is constructed by in-situ anchoring Pt 6 NCs on carbon self-doping g-C 3 N 4 (CCN/Pt 6 NCs) for boosting photocatalytic H 2 evolution activity. Remarkably, the optimized CCN/Pt 6 NCs photocatalyst exhibits high H 2 evolution rate of 6.32 mmol·h −1 ·g −1 and 36.25 mmol·h −1 ·g −1 , which is ≈150.5 and ≈412 times than that of pristine CN under visible light (λ > 420 nm) and full solar spectrum irradiation, respectively, outperforming majority of the reported g-C 3 N 4 -based photocatalysts. Systematic characterizations have revealed that CCN with delocalized electrons and larger the work function is deemed to be a preferable electron-acceptor. Meanwhile, Pt 6 NCs with appropriate HOMO-LUMO level is regarded as an electron-donor. Theoretical and experimental works reveal that the favorable photocatalytic performance of CCN/Pt 6 NCs heterojunction is mainly attributed to the giant internal electric field induced donor–acceptor interaction, which achieves Z-scheme charge transfer mechanism. This work opens up new insights for rational fabrication of metal-free g-C 3 N 4 based photocatalysts to boost the solar energy conversion.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

MoSe2-NiSe dual co-catalysts modified g-C3N4 for enhanced photocatalytic H2 generation

Yan An,Xiaoping Hu,Xinyu Wang,Jian Tian

Solar energy conversion into hydrogen (H 2 ) energy has attracted much attention. However, the low light utilization rate and fast carrier recombination of photocatalysts extremely limit the practical application of photocatalytic H 2 production. In this paper, MoSe 2 -NiSe with abundant active sites and interfacial electronic structures as dual co-catalysts were assembled on g-C 3 N 4 nanosheets (NSs) vis a solvothermal reaction process. MoSe 2 -NiSe/g-C 3 N 4 NSs composite exhibited improved light absorption and photoelectrochemical properties. The photocatalytic H 2 production rate of MoSe 2 -NiSe/g-C 3 N 4 composite achieved 2379.04 μmol·h −1 ·g −1 , which is 99.25, 1.44, and 3.67 times those of pure g-C 3 N 4 nanosheets (23.97 μmol·h −1 ·g −1 ), MoSe 2 /C 3 N 4 (1654.57 μmol·h −1 ·g −1 ), and NiSe/C 3 N 4 (649.08 μmol·h −1 ·g −1 ), respectively. The apparent quantum efficiency (AQE) value of MoSe 2 -NiSe/g-C 3 N 4 achieved 4.07 % under light at λ = 370 nm. The corresponding characterization and experiments proved that 2D ultrathin g-C 3 N 4 NSs with a large surface area and short charge-transfer distance could facilitate light scattering and the transport of photoexcited electrons. MoSe 2 -NiSe, as a dual co-catalyst, showed strong electronic synergistic interaction between the interfaces, thus improving the conductivity and promoting the electron transfer process.

CAS / MDL: 16940-66-2
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Ultra-thin nanosheet assembled 3D honeycomb-like Zn0.5Cd0.5S for boosting photocatalytic H2 evolution

Wenjuan Fan,Hui Chang,Wenju Pang,Yufeng Li,Chuanhai Xiao,Yan Jiang,Zhiqiang Jiang,Guangfu Yin

Designing photocatalysts with excellent morphology from MOF is a promising strategy to improve photocatalytic H 2 evolution. Herein, a three-dimensional (3D) honeycomb-like Zn 0.5 Cd 0.5 S -140 assembled by ultra-thin nanosheets with an average thickness of about 1.5 nm was constructed using a novel 3D metal–organic framework (namely PZH-139) as template. Notably, the micromorphology could be tuned and the balance between conduction band (CB) position and band gap could achieve by adjusting the Zn/Cd molar ratio of Zn x Cd 1-x S. In a series of Zn x Cd 1-x S -140 photocatalysts derived from MOF, Zn 0.5 Cd 0.5 S -140 exhibited the highest hydrogen evolution rate (26.32 mmol h −1 g −1 ) by visible-light-driven with an apparent quantum efficiency (AQE) of 29.92 %, which was 6, 11 and 23 times higher than that of I-Zn 0.5 Cd 0.5 S (irregular morphology Zn 0.5 Cd 0.5 S), S-Zn 0.5 Cd 0.5 S (spherical Zn 0.5 Cd 0.5 S) and B-Zn 0.5 Cd 0.5 S (bulk Zn 0.5 Cd 0.5 S) prepared by traditional non-MOFs derived-methods, respectively. The excellent photocatalytic performance could be attributed to the synergism of the larger specific surface area, the balance between CB position and band gap, rapid carriers transfer and the enhanced light absorption capability. More importantly, this rare strategy for constructing highly efficient ultra-thin nanosheet assembled 3D honeycomb-like Zn 0.5 Cd 0.5 S -140 derived from MOF can flourish the design ideas of photocatalysts with specific excellent morphology.

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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Dual cocatalyst modified CdS achieving enhanced photocatalytic H2 generation and benzylamine oxidation performance

Binshu Sun,Jianhong Zheng,Dewu Yin,Huile Jin,Xin Wang,Quanlong Xu,Aili Liu,Shun Wang

Cocatalyst can greatly facilitate the charge separation efficiency and decrease the activation barrier of a specific reaction, thus contributing the improved photocatalytic performance. Herein, PdS/CdS/MoS 2 was synthesized via a facile microwave-assisted approach. Owing to the coexistence of PdS and MoS 2 , respectively serving as oxidation and reduction cocatalyst, PdS/CdS/MoS 2 displayed enhanced photocatalytic performance in both hydrogen production (6610 μmol·g −1 ·h −1 ) and benzylamine oxidation (87% conversion) in comparison with the individual and binary composite counterparts. The improved photocatalytic activity was mainly attributed to the high charge separation efficiency and lowed activation barrier. Furthermore, the introduction of PdS can timely extract photogenerated holes from CdS, which effectively inhibits the photo-corrosion of CdS, endowing it with high stability. This work paves the way for developing efficient chalcogenide photocatalysts.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Sustainable biomass upgrading coupled with H2 generation over in-situ oxidized Co3O4 electrocatalysts

Chunlin Chen,Zhenqiang Zhou,Jing Liu,Bin Zhu,Hualei Hu,Yong Yang,Guoxin Chen,Minrui Gao,Jian Zhang

Substituting overall water splitting with simultaneous biomass upgrading and H 2 evolution has drawn tremendous attention due to the lower energy barrier and higher safety. Developing a cheap, efficient, and durable electrocatalyst with dual function is crucial to this novel coupling system. Herein, we propose the in-situ electrochemical tuning nonporous CoS x to hydrangea-like Co 3 O 4 as a highly effective versatile electrocatalyst for the first time. Due to the defective structures and abundant electroactive sites, the Co 3 O 4 catalyst achieved a complete conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) with 93.2% yield and 92.9% faradaic efficiency (FE), as well as a pure hydrogen evolution with 99.8% FE. Interestingly, it harvested a better performance with 95.8% FDCA yield for electro-oxidation of the more stable 2,5-bis(hydroxymethyl)furan (BHMF). Finally, a solar-driven integration reaction was constructed for the first time using the photovoltaic electrocatalysis (PVEC) of BHMF for the efficient and sustainable production of FDCA and H 2 .

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CERAMICS INTERNATIONAL · 2022 · IF 5.532

High performance H2 sensor based on rGO-wrapped SnO2–Pd porous hollow spheres

Tong Qiu,Shiyu Zhou,Jiapeng Ji,Gu Wu,Wenjun Yan,Min Ling,Chengdu Liang

Hydrogen (H 2 ) sensors based on metal oxide semiconductors (MOS) are promising for many applications such as a rocket propellant, industrial gas and the safety of storage. However, poor selectivity at low analyte concentrations, and independent response on high humidity limit the practical applications. Herein, we designed rGO-wrapped SnO 2 –Pd porous hollow spheres composite (SnO 2 –Pd@rGO) for high performance H 2 sensor. The porous hollow structure was from the carbon sphere template. The rGO wrapping was via self-assembly of GO on SnO 2 -based spheres with subsequent thermal reduction in H 2 ambient. This sensor exhibited excellently selective H 2 sensing performances at 390 °C, linear response over a broad concentration range (0.1–1000 ppm) with recovery time of only 3 s, a high response of ∼8 to 0.1 ppm H 2 in a minute, and acceptable stability under high humidity conditions (e. g. 80%). The calculated detection limit of 16.5 ppb opened up the possibility of trace H 2 monitoring. Furthermore, this sensor demonstrated certain response to H 2 at the minimum concentration of 50 ppm at 130 °C. These performances mainly benefited from the special hollow porous structure with abundant heterojunctions , the catalysis of the doped-PdO x , the relative hydrophobic surface from rGO, and the deoxygenation after H 2 reduction.

CAS / MDL: 8000-41-7
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Materials Today Chemistry · 2022 · IF 7.613

Ferrocene-based hypercrosslinked polymers derived from phenolic polycondensation with unexpected H2 adsorption capacity

Q. Peng,H. Zhao,R. Wang,X. Cao,H. Liu,Q. Liu

Metal-doped porous organic polymers often display unique properties for applications in gas uptake owing to the incorporation of the metal elements in the polymer networks . In this study, a series of novel ferrocene-based hypercrosslinked polymers were prepared by phenolic polycondensation (Fc-PR-HCPs). To generate the hypercrosslinked polymers, 1,1′-ferrocenedicarboxaldehyde (Fc(CHO) 2 ) and bisphenol A (BPA) were used as the building blocks. The maximum value of BET and micropore surface area is determined to be 1111.4 and 487.4 m 2 /g for Fc-PR-HCP3. A significant H 2 adsorption capacity of 3.11 wt% was achieved for Fc-PR-HCP3 at 77 K/1.0 bar, which was noted to be higher than the porous organic polymers with even higher BET surface area value. The high micropore surface area value and the adsorption sites (aromatic rings and metal ion-active sites) provided by two building blocks were used to explain the significant H 2 adsorption capacity successfully. Overall, the findings from this study indicate that Fc-PR-HCPs highlighted prospective applications in the field of H 2 capture.

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