Surfaces and Interfaces
·
2025
·
IF 6.3
Dawson Wai-Shun Suen,Yujie Yan,Eugene Yin-Cheung Wong,Xiao-Ying Lu,Jiajun Chen,Chi-Wing Tsang,Chunzhen Yang,Shaobo Ouyang
This study investigated the long-term stability of cobalt (Co) and manganese nitride (Mn 4 N) nanoclusters in the catalytic hydrolysis of a promising hydrogen (H 2 ) storage material, ammonia borane (H 3 NBH 3 ; AB), to release H 2 . It was previously found that Co nanoparticle/Co single-atom catalysts (Co NP/Co SACs) anchored on carbon nanotubes (CNT) exhibited excellent reactivity and stability towards AB hydrolysis and high performance in the H 2 evolution reaction in alkaline media. Therefore, the current study synthesised CoMn 4 N/Co-Mn-N x -CNT-200-800, a CoMn-based catalyst with Co and Mn 4 N nanocluster active sites, and examined its performance in AB hydrolysis. CoMn 4 N/Co-Mn-N x -CNT-200-800 generated three equivalents of H 2 from AB within 5 min, outperforming the catalytic activity of previously reported Co NPs/Co SACs. Moreover, CoMn 4 N/Co-Mn-N x -CNT-200-800 maintained over 90% of its initial activity after 50 cycles of AB hydrolysis. This exceptional long-term stability is attributable to CoMn 4 N/Co-Mn-N x -CNT-200-800 bearing Co/Mn 4 N nanoclusters that were strongly adhered onto graphitic layers, thereby preventing metal-atom aggregation and leakage during AB hydrolysis. Thus, CoMn 4 N/Co-Mn-N x -CNT-200-800 displayed a maximum effective H 2 generation rate of 8372 mL H2 ·g CoMn −1 ·min −1 . These results highlight the potential of dispersed bimetallic nanocluster catalysts, such as CoMn 4 N-based catalysts, for practical and sustainable H 2 generation via AB hydrolysis. In addition, the insights gained from this study can inform the design of highly active and stable non-precious metal-based catalysts for energy-related applications.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2021
·
IF 8.001
Liqing Zhao,Qinghe Wei,Lili Zhang,Yafei Zhao,Bing Zhang
Hydrogen release from catalytic hydrolysis of solid-state ammonia borane (AB) with efficient catalysts is recognized as a safe and compelling strategy to satisfy the ever-increasing demand for clean energy. As a result, exploring extraordinary efficient and inexpensive catalysts for hydrogen generation from AB is urgently desired for practical application. Herein, with the help of bimetallic zeolitic imidazole frameworks (ZnCo-ZIF) template strategy, we successfully decorate non-noble NiCo alloy nanoparticles on ZnCo-ZIF derived porous nitrogen-doped carbon (NC) as a high-efficiency catalyst (NiCo-NC) for hydrogen generation from hydrolysis of AB. Befitting from the abundance of nitrogen in porous carbon, the powerful synergistic effect between Ni and Co and the synergistic effect between the metallic alloy and the supporting substrate, the as-prepared NiCo-NC nano-catalyst displays distinguished catalytic performance with a high total turnover frequency (TOF) of 35.2 mol H 2 mo l metal - 1 mi n - 1 in 0.6 M NaOH medium at 298 K. Besides, this catalyst also exhibits good stability and magnetic separability . This work could provide a new insight for the construction of other bimetallic alloy anchoring on porous N-doped carbon carrier for further applications.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2020
·
IF 3.421
Senliang Xi,Peng Zhang,Yuanyi Fu,Kudzaishe Caren Tome,Tonghuan Zhang,Shixue Zhou,Youmin Guo,Hao Yu
In this work, two kinds of zeolites MCM-22 and SAPO-34 were synthesized by the hydrothermal method. The mixture systems of NaBH4 and different mass percentages of zeolite were prepared by ball milling, with no reaction between NaBH4 and the zeolite during the process, as shown by X-ray diffraction analysis. Thermal decomposition of NaBH4 and NaBH4 + zeolite for hydrogen release was investigated by temperature-programmed desorption, differential scanning calorimetry, and pressure composition isothermal methods. It is shown that the presence of zeolites can decrease the hydrogen release temperature. In addition, in comparison to pure NaBH4, whose peak temperature of hydrogen release was 566.8 °C, the peak temperatures of NaBH4 + MCM-22 (1:1) and NaBH4 + SAPO-34 (1:1) decreased to 510.0 and 505.2 °C, respectively. Moreover, the addition of zeolite can improve the hydrogen release kinetics of NaBH4 and when catalyzed by MCM-22 and SAPO-34 can release 2.31 and 3.76 wt. % H2 in 15 h, respectively. Furthermore, SAPO-34 with the larger specific surface area had a better nanoconfinement effect to catalyze hydrogen release of NaBH4 than that of MCM-22.
研究领域:
材料化学
·
能源化学
·
纳米催化
·
储氢材料
·
物理化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Weifeng Chen,Guo Lv,Jinrun Fu,Haiyan Ren,Jialu Shen,Jie Cao,Xiang Liu
Achieving the controlled release of H2 through an effective approach still faces many challenges. Herein, high-quality graphene quantum dots (GQDs) are synthesized from a new precursor, 1,2,4-trihydroxy benzene, and a multifunctional platform of Rh@GQDs is further developed for the controlled H2 evolution upon the hydrolysis of NH3BH3 (AB). More importantly, the designing concepts of multistep and stepless speed controls have been introduced in the domains of both H2 evolution for the first time. Through a novel designing protocol, the rate of H2 evolution can be freely regulated and constantly varied on demand by means of chelation between Zn2+ and ethylene diamine tetraacetic acid (EDTA). The density functional theory calculation indicates that Zn2+ has the priority to be adsorbed onto Rh(100) due to its larger adsorption energy (107.98 kcal·mol–1) than that of AB (36.36 kcal·mol–1). A controlling mechanism is presented such that Zn2+ will cover the active sites of the nanocatalyst to prevent the H2 evolution, and EDTA can chelate Zn2+ to reactivate the nanocatalyst for the production of H2, greatly facilitating use of this strategy in other catalytic reactions. Moreover, it is demonstrated that the protocol is equally valid for diverse hydrogen storage materials. Therefore, this work not only establishes whole new concepts for the controlled production of H2 but also explains their mechanism, thus remarkably advancing the utilization of H2 energy and significantly enlightening the controlled process of catalysis.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Fuhua Xu,Yanlan Wang,Changlong Wang,Wenkai Huang,Xiang Liu
In despite of significant progresses have been accomplished in the programming and development of updated and efficient nana-catalysts for H 2 production from a wide variety of chemical hydrogen storage materials. However, it is a practical matter of the utmost importance to develop the “on-off” control for on demand H 2 release in the cause of effectively and safely producing, carrying and depositing H 2 gas. Herein, we have first designed and synthesized a sequence of carbon nanosphere (CNS)-stabilized bimetallic PtNi nanoparticles (PtNi/CNS), by stabilization of nearly monodispersed PtNi bimetallic nanoparticles onto the surface of carbon nanosphere, for the highly selective and efficient on-demand H 2 release upon the dehydrogenation of hydrous hydrazine. Then, the optional nanocatalyst Pt 1 Ni 1 /CNS exhibits the highest catalytic performance in hydrogen production from dehydrogenation of hydrous hydrazine, with 100 % H 2 selectivity and the turnover frequency (TOF) of 3928 mol (H 2 )·mol cat −1 ·h −1 at 50 °C. The detailed physical characterizations have confirmed that the superior catalytic performance of Pt 1 Ni 1 /CNS in the H 2 release upon hydrous hydrazine dehydrogenation is attributed to the electronic interaction and synergistic effect between Ni and Pt. More importantly, the highly selective “on-off” control for demand-based H 2 release upon the dehydrogenation of hydrous hydrazine is successfully realized by pH regulation.
研究领域:
材料科学
·
催化化学
·
能源存储与转换
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2018
·
IF 4.229
Ying-Hua Zhou,Zhiyan Zhang,Suqin Wang,Nicholas Williams,Yong Cheng,Shizhong Luo,Jing Gu
The hydrogen economy is a proposed system that utilizes hydrogen to deliver energy. For the realization of this concept, how to safely, controllably and reversibly store and release hydrogen are critical problems which must be resolved. Metal alloys combined with suitable support materials are widely applied to various catalytic reactions . Here palladium nickel bimetallic nanoparticles doped with cerium oxide on a reduced graphene oxide (rGO) support were prepared by combining metal ion precursors and graphene oxide in a one-pot co-reduction approach. The as-received catalysts were characterized by XRD , TEM, SEM, XPS and ICP-OES, and the results revealed that PdNi-CeO 2 nanoparticles were uniform dispersal on rGO. The as-synthesized PdNi-CeO 2 /rGO had been adopted as a heterogeneous catalyst for the hydrogen evolution from the hydrolysis of ammonia borane (NH 3 BH 3 , AB) at room temperature . Kinetically, the hydrogen-release rate was first-order with the increased concentration of catalysts. The optimized catalyst of Pd 0.8 Ni 0.2 -CeO 2 /rGO with the CeO 2 content of 13.9 mol% exhibited an excellent activity with a turnover frequency value of 30.5 mol H 2 (mol catalyst) −1 min −1 at 298 K, and a low apparent activation energy ( E a ) of 37.78 kJ mol −1 . The robust catalytic performance of the Pd 0.8 Ni 0.2 -CeO 2 /rGO is attributed to the uniform controlled nanoparticle size, the synergic effect between the nanoparticles bimetallic properties, and the effective charge transfer interactions between the metal and support.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2017
·
IF 4.857
Zhujun Zhang,Shiliang Zhang,Qilu Yao,Xiangshu Chen,Zhang-Hui Lu
The catalytic dehydrogenation of hydrazine borane (N2H4BH3) and hydrous hydrazine (N2H4·H2O) for H2 evolution is considered as two of the pivotal reactions for the implementation of the hydrogen-based economy. A reduction rate controlled strategy is successfully applied for the encapsulating of uniform tiny NiPt alloy nanoclusters within the opening porous channels of MOFs in this work. The resultant Ni0.9Pt0.1/MOF core–shell composite with a low Pt content exerted exceedingly high activity and durability for complete H2 evolution (100% hydrogen selectivity) from alkaline N2H4BH3 and N2H4·H2O solution. The features of small NiPt alloy NPs, strong synergistic effect between NiPt alloy NPs and the MOF, and open pore structure for freely mass transfer made NiPt/MIL-101 an excellent catalyst for highly efficient H2 evolution from N2H4BH3 or N2H4·H2O.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 27
·13694-13701
·
IF 11.301
Wei Wang,Xiaoling Hong,Qilu Yao,Zhang-Hui Lu
In this work, mesoporous N-doped carbon (MNC) materials have been successfully prepared by a nanocasting route using SBA-15 as the template and ethylenediamine (EDA) and carbon tetrachloride (CTC) as carbon nitride precursors. The specific surface area and pore size of the MNC, as well as the C/N content are strongly dependent on the pyrolysis temperature. The as-obtained MNC-supported NiPt nanoparticles (NPs) were used as efficient catalysts toward complete dehydrogenation of hydrazine borane (HB) in alkaline solution at room temperature. Among all the catalysts investigated, the Ni60Pt40/MNC-800 nanocomposites (NCs) show the highest catalytic activity and 100% hydrogen selectivity. The total turnover frequency (TOF) of Ni60Pt40/MNC-800 NCs reached 1111 h−1 at room temperature, the highest activity among all catalysts reported to date. The superior catalytic properties were possibly a result of the electronic interaction between Ni and Pt, the synergistic effects of the NiPt NPs and MNC support, the ordered pore structure for free mass transfer and the small-sized metal NPs.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Jinbo Yang,Shengqi Lin,Chunhe Li,Kuankuan Ren,Qiufeng Ye,Weidong Dou
Utilizing photocatalytic technology to efficiently convert biomass-derived compounds into value-added chemicals and release hydrogen gas can effectively address energy and environmental issues. For this purpose, we fabricated a series of NiMoS4/Zn0.6Cd0.4S nanocomposites through a simple two-pot hydrothermal treatment. Dexterously, the photoexcited electrons and holes can be simultaneously utilized to participate in a photocatalytic redox reaction, effectively achieving the oxidation of furfuryl alcohol while cooperating with H2 evolution. The hydrogen evolution rate of 10%-NiMoS4/Zn0.6Cd0.4S nanocomposite in 1.50 vol % furfuryl alcohol aqueous solution is as high as 289.5 μmol·h–1, which is approximately 2895 and 41 times higher than that of pure NiMoS4 and Zn0.6Cd0.4S, respectively. Meanwhile, after 13 cycles of photocatalytic reaction, the conversion efficiency and selectivity of converting furfuryl alcohol to furfural are 68.5% and 94.0%, respectively. This photocatalyst also shows high photocurrent, low impedance, and efficient photogenerated carrier separation and transport properties, which can be attributed to the establishment of an ohmic junction between NiMoS4 and Zn0.6Cd0.4S. It is anticipated that this work can provide inspiration for the effective conversion of biomass-derived platform chemicals into high-value chemicals through visible-light-driven photocatalytic technology.
研究领域:
能源科学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2022
·
IF 10.319
Yang Zhao,Tong Li,Haixiang Huang,Tingting Xu,Bogu Liu,Bao Zhang,Jianguang Yuan,Ying Wu
MgH 2 has a high theoretical hydrogen production capacity and mild conditions for hydrogen production by hydrolysis, so it is suitable as an ideal hydrogen source for fuel cells. However, with the progress of the hydrolysis reaction, MgH 2 is impeded from reacting further by the continuous deposition of magnesium hydroxide on its surface, resulting in low hydrogen yield and slow reaction kinetics. In the present work, a highly efficient NiCo bimetallic synergistic catalysis is developed to improve the hydrolysis performance of MgH 2 . The MgH 2 -8 wt% NiCo@C composite ball-milled for 5 h achieves nearly 100% hydrogen desorption efficiency within 15 min in 0.05 mol L –1 MgCl 2 solution. Because the interaction between Ni and Co on the surface of MgH 2 can form a channel for rapid hydrogen evolution, which hinders the continuous formation of the Mg(OH) 2 passivation layer and promotes the hydrolysis reaction of MgH 2 . This is very important for the implementation of MgH 2 hydrolysis to produce hydrogen in the future.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE CHEMICAL LETTERS
·
2024
·
IF 9.4
Shuai Li,Liuting Zhang,Fuying Wu,Yiqun Jiang,Xuebin Yu
Hydrogen, as a cheap, clean, and cost-effective secondary energy source, performs an essential role in optimizing today's energy structure. Magnesium hydride (MgH 2 ) represents an attractive hydrogen carrier for storage and transportation, however, the kinetic behavior and operating temperature remain undesirable. In this work, a dual-phase multi-site alloy (MsA) anchored on carbon substrates was designed, and its superior catalytic effects on the hydrogen storage properties of MgH 2 were reported. Mechanism analysis identified that multi-site FeNi 3 /NiCu nanoalloys synergistically served as intrinsic drivers for the striking de/hydrogenation performance of the MgH 2 -MsA systems. Concretely, the unique multi-metallic site structure attached to the surface of MgH 2 provided substantial reversible channels and accessible active sites conducive to the adsorption, activation, and nucleation of H atoms. In addition, the coupling system formed by FeNi 3 and NiCu dual-phase alloys further enhanced the reactivity between Mg/MgH 2 and H atoms. Hence, the onset dehydrogenation temperature of MgH 2 + 5 wt% MsA was reduced to 195°C and the hydrogen desorption apparent activation energy was reduced to 83.6 kJ/mol. 5.08 wt% H 2 could be released at 250°C in 20 min, reaching a high dehydrogenation rate of 0.254 wt% H 2 /min, yet that for MgH 2 at a higher temperature of 335°C was only 0.145 wt% H 2 /min. Then, the dehydrogenated MgH 2 -MsA sample could absorb hydrogen from room temperature (30°C) and charge 3.93 wt% H 2 at 100°C within 20 min under 3.0 MPa H 2 pressure. Benefiting from carbon substrates, the 5 wt% MsA doped-MgH 2 could still maintain 6.36 wt% hydrogen capacity after 20 cycles. In conclusion, this work provides experimental rationale and new insights for the design of efficient catalysts for magnesium-based solid-state hydrogen storage materials.
研究领域:
材料科学
·
能源存储
·
催化
·
氢能技术
✓ 已验证
DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2025
·Vol. 99
·期 5
·991-1000
·
IF 0.8
Ji Xiang,Zeng Lingyun,Wang Lingjuan,Wang Zhipeng,Zhu Hailong,Lu Yanzhen,Rao Richuan,Wang Fangkuo
— It is of great significance to prepare high-performance non-precious metal catalysts for hydrogen evolution from the ammonia borane (NH 3 BH 3 , AB). Here, a series of cost-effective and high-performing Ag–Co 3 O 4 nanocatalysts were prepared using AgNO 3 and Co(NO 3 ) 2 ⋅6H 2 O as precursors. The influence of varying doping amounts of Ag atoms (10 mg AgNO 3 , 20 mg AgNO 3 , 40 mg AgNO 3 , 60 mg AgNO 3 ) and heat treatment temperatures (300, 400, 500, 600°C) on the catalytic activity of the Ag–Co 3 O 4 nanocatalysts for AB hydrolysis was investigated. The obtained results reveal that the Ag–Co 3 O 4 nanocatalysts exhibit a well-defined nano-flower morphology with homogeneous distribution of silver atoms over the Co 3 O 4 surface. Moreover, an evident electronic synergy between Ag and Co 3 O 4 is observed. The 20-Ag–Co-500 catalyst (doped with 20 mg of AgNO 3 and subjected to heat treatment at 500°C) exhibits exceptional catalytic activity towards AB hydrolysis (TOF = 348.03 \({\text{mo}}{{{\text{l}}}_{{{{{\text{H}}}_{{\text{2}}}}}}}\) min –1 \({\text{mol}}_{{{\text{Ag}}}}^{{ - 1}}\) and E a = 56.20 kJ/mol).
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）