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FUEL · 2025 · IF 7.5

Construction of NiAl-LDH/Mn0.5Cd0.5S heterostructure for enhancing photocatalytic H2 evolution

Yunxia Luo,Yongping Luo,Chao Liu,Wenzhen Qin,Yuhua Dai,Yu Xie,Xiu Wang,Jiansheng Zhang

Plumbing and devising photocatalysts for high photocatalytic hydrogen production is still a major challenge. In this study, the NiAl-LDH/Mn 0.5 Cd 0.5 S heterostructure composites are prepared by hydrothermal method. When the loading weight of NiAl-LDH is 20 wt%, NiAl-LDH/Mn 0.5 Cd 0. 5S composites has the excellent ability to separate photogenerated charge carriers under visible light. Meantime, the NiAl-LDH/Mn 0.5 Cd 0.5 S composites possess prominent photocatalytic hydrogen production rates of 55.9 mmol·h −1 ·g −1 , which is 7.5 times of pure Mn 0.5 Cd 0.5 S and 25 times of NiAl-LDH. According to the data, the photocatalytic mechanism of electron-holes movement over NiAl-LDH/Mn 0.5 Cd 0.5 S composites is unlocked. This work offers a reference for designing novel heterojunction for photocatalytic production of H 2 .

研究领域: 材料科学 · 光催化
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-11 · IF 14.7

Induced dipole moments in amorphous ZnCdS catalysts facilitate photocatalytic H2 evolution

Wang Xin,Liu Boyan,Ma Siqing,Zhang Yingjuan,Wang Lianzhou,Zhu Gangqiang,Huang Wei,Wang Songcan

Amorphous semiconductors without perfect crystalline lattice structures are usually considered to be unfavorable for photocatalysis due to the presence of enriched trap states and defects. Here we demonstrate that breaking long-range atomic order in an amorphous ZnCdS photocatalyst can induce dipole moments and generate strong electric fields within the particles which facilitates charge separation and transfer. Loading 1 wt.% of low-cost Co-MoS x cocatalysts to the ZnCdS material increases the H 2 evolution rate to 70.13 mmol g −1 h −1 , which is over 5 times higher than its crystalline counterpart and is stable over the long-term up to 160 h. A flexible 20 cm × 20 cm Co-MoS x /ZnCdS film is prepared by a facile blade-coating technique and can generate numerous observable H 2 bubbles under natural sunlight, exhibiting potential for scale-up solar H 2 production.

研究领域: 材料科学 · 能源化学
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JOURNAL OF POWER SOURCES · 2024 · IF 8.1

Low-cost H2/K+ hybrid batteries for large-scale energy storage

Shuang Liu,Ying Wang,Zhengxin Zhu,Jingwen Xu,Zuodong Zhang,Kai Zhang,Song Jin,Zehui Xie,Taoli Jiang,Xiaoyang Wang,Zaichun Liu,Jinghao Chen,Qia Peng,Muhammad Sajid,Touqeer Ahmad,Wei Chen

Rechargeable hydrogen gas batteries are gaining significant attention as a highly reliable electrochemical energy storage technology. However, the high costs of both cathode and anode limit their widespread applications. Here, we demonstrate a low-cost H 2 /K + hybrid battery using Fe–Mn-based Prussian white - K 2 · 74 Mn[Fe(CN) 6 ] 0.90 ·0.13H 2 O (KMF) as cathode and non-noble metal high entropy alloy (NNM-HEA) as anode. It demonstrates a high capacity of 146.1 mAh g −1 at 1 A g −1 with excellent rate performance and stability. Even with a ∼7-fold increase in active loading of the KMF cathode, the capacity of the H 2 /K + battery remains as high as 100.5 mAh g −1 . Furthermore, a low-cost H 2 /K + hybrid battery using our newly developed NNM-HEA based hydrogen catalytic anode is successfully fabricated, which shows an extended capacity with a retention of 90% after 1200 cycles. This work will pave the way for designing low-cost electrode materials for high-performance, large-scale energy storage hydrogen gas batteries.

CAS / MDL: 872-50-4
研究领域: 材料科学 · 能源存储技术
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Chemical Science · 2019 ·Vol. 10 ·期 45 ·10640-10646 · IF 9.556

Synthesis of ethanol from aryl methyl ether/lignin, CO2 and H2

Jingjing Zhang,Qingli Qian,Ying Wang,Bernard Baffour Asare Bediako,Jiang Yan,Buxing Han

Currently, ethanol is produced via hydration of ethene or fermentation of foods. Lignin and CO2 are abundant, cheap and renewable feedstocks. Synthesis of ethanol using the lignin or its derivatives is of great importance, but is a great challenge and has rarely been reported. Herein, we propose a route to synthesize ethanol from CO2, H2, and lignin or various aryl methyl ethers, which can be derived from lignin. The reaction could be effectively conducted using Ru–Co bimetallic catalyst and the TON of ethanol could reach 145. Interestingly, ethanol was the only liquid product when lignin was used. A series of control experiments indicate that ethanol was formed via cleavage of aryl ether bond, reverse water gas shift (RWGS) reaction, and C–C bond formation. This protocol opens a way to produce ethanol using abundant renewable resources.

研究领域: 化学工程 · 可再生资源利用
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Inorganic Chemistry Frontiers · 2022 ·Vol. 9 ·期 9 ·1943-1955 · IF 7.779

Efficient H2 evolution on Co3S4/Zn0.5Cd0.5S nanocomposites by photocatalytic synergistic reaction

Yang Yang,Xiuzhen Zheng,Jiafang Liu,Zhulin Qi,Tianyue Su,Chun Cai,Xianliang Fu,Sugang Meng,Shifu Chen

To achieve high photocatalytic efficiency of H2 evolution, promoting the utilization rate of photogenerated charge carriers by photocatalytic synergistic reaction is an efficient strategy. In this work, Co3S4/Zn0.5Cd0.5S nanocomposites with Co3S4 derived from ZIF-67 were successfully prepared through a simple hydrothermal method. Under visible light irradiation, Co3S4/Zn0.5Cd0.5S exhibited high photocatalytic activities in a H2 production system coupled with selective oxidation of benzyl alcohol. Moreover, 3% Co3S4/Zn0.5Cd0.5S showed the optimal activity (7.67 mmol g−1 h−1), greatly improved compared to that of Zn0.5Cd0.5S (1.62 mmol g−1 h−1). The reasons for the improved photocatalytic performance were seriously investigated by a variety of measurements and can be attributed to the enhanced visible light absorption and more efficient electron–hole pair separation. This study provides a good strategy to construct photocatalysts with metal–organic frameworks (MOFs) and efficient charge separation for highly efficient H2 production.

研究领域: 材料科学 · 能源科学
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CHEMICAL ENGINEERING & TECHNOLOGY · 2018 ·Vol. 41 ·期 4 ·867-874 · IF 1.588

Correlation between Liquid Product Distribution and H2 Selectivity in Lignin Depolymerization

Jing Yang,Shaotong Liu,Chunze Liu,Yuanyuan Wang,Liyi Dai

Despite the vast potential for the depolymerization of kraft lignin in supercritical systems, selective access to desired renewable products remains a very challenging target. Catalytic depolymerization of kraft lignin was carried out in an isopropanol-water mixture system over a Rh/La 2 O 3 /CeO 2 -ZrO 2 catalyst. The H 2 selectivity was adjusted by changing the proportions of isopropanol and water. The introduction of formic acid was more helpful to extend the selectivity range. A correlation was established between liquid product distribution and H 2 selectivity. It was used for predicting the composition of the liquid oil by H 2 selectivity or, optionally, for converting kraft lignin to the desired liquid products. This correlation was applicable to different solvents, temperatures, and catalysts.

研究领域: 化学工程 · 可再生资源
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NANOTECHNOLOGY · 2014 ·Vol. 25 ·期 21 ·215401 · IF 3.672

Superior H2 production by hydrophilic ultrafine Ta2O5 engineered covalently on graphene

Lin Mao,Shenmin Zhu,Jun Ma,Dian Shi,Yixin Chen,Zhixin Chen,Chao Yin,Yao Li,Di Zhang

A H2O2-mediated hydrothermal method was developed for the fabrication of hydrophilic Ta2O5/graphene composite. The composite shows a superior H2 productivity, up to 30 mmol g−1 h−1 when used as a photocatalyst for water splitting, corresponding to an apparent quantum efficiency of 33.8% at 254 nm. This superior performance is due to the hydrophilic nature of the composite and more importantly due to the ultrafine Ta2O5 nanoparticles (about 4.0 ± 1.5 nm) which are covalently bonded with the conductive graphene. The hydrophilic property of the composite is attributed to the use of H2O2 in the hydrothermal process. The ultrafine size of the Ta2O5 particles which are covalently bonded with the graphene sheets is attributed to the use of sonication in the synthesis process. Furthermore, the hydrophilic Ta2O5/Gr composite is durable, which is beneficial to long term photocatalysis. The strategy reported here provides a new approach to designing photocatalysts with superior performance for H2 production.

CAS / MDL: 1314-61-0
研究领域: 材料科学 · 能源化学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Polarization field promoted photoelectrocatalysis for synergistic environmental remediation and H2 production

Yunni Liu,Qian Li,Zichao Lian,Jinchen Fan,Ying Tao,Guisheng Li,Hexing Li

Polarization field introduced photoelectrocatalytic system has been raised and applied for environmental purification and green fuel generation. Herein, we synthesized the Ag 2 O/TiO 2 nanotubes arrays (TNTs) p - n heterojunction photoanodes and innovatively introduced the SrTiO 3 (STO) as a relay to construct a highly stable PEC system. The SrTiO 3 layers with the ferroelectric properties were inserted in the interfaces between p-Ag 2 O and n-TiO 2 , creating a charge-stable polarized electric field thereby maintaining a constant driving force that promoted the effctive separation of electron and hole between SrTiO 3 and TNTs, and prevented the electron transfer from SrTiO 3 to Ag 2 O. Controlling suitable annealing and regulating hydrothermal time could induce SrTiO 3 spontaneous polarization, resulting in effective photoinduced charge separation. Consequently, the as-designed TNTs/STO/Ag 2 O photoanodes exhibited excellent PEC activity and stability (>40 h) for both persistent organic pollutants degradation and synergistic hydrogen evolution owing to the strengthened charge carrier capture ability of solar light and improved photocurrent density.

研究领域: 环境科学 · 材料科学 · 能源科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

Cocatalyst decorated ZnIn2S4 composites for cooperative alcohol conversion and H2 evolution

Chang-Long Tan,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu

Highly efficient photodriven conversion from biomass-derived platform chemicals to value-added chemical feedstocks and clean fuel hydrogen (H 2 ) possesses immense potential to cope with the existing energy and environmental problems. We herein report a facile approach combining hydrothermal method and photodeposition method for fabricating diverse sulfide-based cocatalysts (MoS 2 , NiS and WS 2 ) decorated ZnIn 2 S 4 (ZIS) for simultaneous exploitation of photogenerated electrons and holes, effectively achieving the oxidation of furfuryl alcohol (FOL) cooperative with H 2 evolution in one photoredox cycle. The results show the optimal binary MoS 2 -ZIS composites can obtain almost 7 times yield of products (furfural and H 2 ) as high as that of blank ZIS. Notably, compared with previous reports in literatures, our present MoS 2 -ZIS shows the best performance in this photoredox dual reaction. As a relay station for electrons, cocatalysts facilitate the separation and transfer of photogenerated charge carriers in the composites, therefore prominently improving the photocatalytic performance. We anticipate that the present work can offer insights to guide the design of photoredox reaction systems for efficient valorization of biomass-derived platform chemicals.

研究领域: 化学工程 · 材料科学 · 环境科学 · 能源科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2023 · IF 4.2

Laminar MoS2 Nanosheets Embedded into Organosilica Membranes for Efficient H2 Separation

Xiuxiu Ren,Fukang Shi,Meng Guo,Jing Zhong,Rong Xu,Zheng Yao,Dongliang Jin,Ting Qi,Liang Zhou

Two-dimensional (2D) molybdenum disulfide (MoS2) with a unique action on H2 was incorporated into 1,2-bis(triethoxysilyl)ethane (BTESE)-derived bridged microporous organosilica networks to form a composite membrane for H2 separation by a sol–gel method. Due to their opposite ζ-potentials, a continuous surface without lamellar boundary defects was formed between BTESE sols derived by the hydrolysis–polymerization reaction and MoS2 nanosheets. When the MoS2 content increased in BTESE networks, the H2 permeance showed an overall increasing trend in the range of 1.85–2.89 × 10–7 mol·m–2 s–1 Pa–1 (552–864 GPU), which was higher than that of pristine BTESE membrane with the H2 permeance of 491 GPU. In addition, optimized MoS2/BTESE membranes showed a much higher H2/N2 permselectivity of 129 than that of the pristine BTESE membrane of 17 at 100 °C. The synergistic effect of BTESE and MoS2 nanosheets plays an important role. Through adsorption isotherm test and diffusivity as well as energy calculation, BTESE networks became denser by nonporous MoS2 addition that prevented N2 from passing, while H2 was promoted with excellent adsorption on charged edges of MoS2, resulting in improved H2 separation performance both in permeance and selectivity. This provides an attractive mechanism for hydrogen separation.

CAS / MDL: 1344-28-1
研究领域: 材料科学 · 化学工程
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Zn0.1Cd0.9S/NiS heterojunction photocatalysts for enhanced H2 production and glucose conversion

Yuan-Sheng Shen,Fang-Yuan Bai,Ke Wei,Xin-Ling Wang,Jun Chen,Ze-Yu Jiang,Jing Liu,Zhi-Yi Hu,Li-Hua Chen,Yu Li,Bao-Lian Su

The well-designed photocatalyst is a reasonable strategy to realize the photocatalytic H 2 -production and biomass conversion. In this work, the noble-metal-free Zn 0.1 Cd 0.9 S/NiS (SNS) composite was successfully prepared by in-situ chemical bath deposition of NiS nanoparticles on Zn 0.1 Cd 0.9 S (ZCS) nanorods surface for photocatalytic H 2 -production using glucose as electron donors for effective utilization of holes. Our results show that the synergistic effect of NiS and ZCS largely improves the absorption and utilization of light, and the photogenerated electrons transfer from NiS to ZCS to effectively separate the photogenerated carriers for the enhanced photocatalytic H 2 -production as the one-dimensional nanorods is conducive to the transmission of photogenerated carriers. The optimized catalyst (SNS20) has the highest H 2 production rate (12.77 mmol·g −1 ·h −1 ), which is 6.7 times that of pure ZCS nanorods. In particular, its apparent quantum efficiency (AQE) at 350 nm reaches 12.74%. The glucose conversion increases from 25.7% to 49.9% and lactic acid selectivity reaches 95%. During three cycles, the SNS20 shows the stable H 2 -production rate, which remains 12 mmol·g −1 ·h −1 after three cycles. And the glucose conversion still remains above 40%. This work provides a reasonable strategy for designing heterojunction photocatalyst to improve the performance for the synergy of photocatalytic H 2 -production and biomass conversion.

研究领域: 材料科学 · 环境科学
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iScience · 2023 · IF 5.8

Selective and efficient H2 evolution upon NH3BH3 hydrolysis at subzero temperatures

Qing Zhang,Chen Fang,Yanlan Wang,Xiang Liu

Summary In the winter months, the temperature in most of the Earth stays below 0°C; the average temperature in winter at the South Pole is about −60°C. Therefore, it is urgent to develop efficient catalytic systems for selective and efficient H 2 evolution upon NH 3 BH 3 hydrolysis at subzero temperatures. For solving the freezing issue of water at below 0°C, herein, we have employed a facile and surfactant-free approach to synthesize M-Pt/C nanocomposites (M = Pd, Rh, Ru, Ni, Cu, or Fe), by the alloying of commercial Pt/C with Pd, Rh, Ru, Cu, Ni, or Fe for selective and efficient H 2 evolution upon NH 3 BH 3 hydrolysis in saline solution at below 0°C, even at −15°C. In addition, NH 3 BH 3 hydrolysis over Pd-Pt/C in the saturated NaCl solution is utilized not only for safe hydrogen production but also for its in situ hydrogenation reduction in organic chemistry, which could avoid using dangerous hydrogen cylinders.

CAS / MDL: 7440-06-4
研究领域: 化学 · 材料科学 · 能源研究
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