FUEL
·
2025
·
IF 7.5
Yu-Yang Cao,Yi Xiong,Xiao-Li Zhang,Xin-Xin Guan,Xiu-Cheng Zheng
Developing a convenient and environmental-friendly catalyst preparation method is of great significance, while the catalytic hydrolysis of ammonia borane (NH 3 BH 3 , AB) is an effective in-situ hydrogen production strategy but faces many challenges including the absence of practicable catalysts. In this study, Ru nanoparticles are tightly encapsulated into the framework of chitosan (CS)-derived carbon aerogel (CCA) through a facile ice-crystal template method combined with one-step direct calcination without using any additional chemical activators. The exciting coordination between Ru 3+ and the N/O-based functional groups of CS in aqueous solution, the hierarchical porous structure of CCA and the self-doped N/O favor the tight and high dispersion of Ru NPs, facilitate mass transfer, as well as improve the hydrophilicity of the resulting catalysts. Therefore, the resulting catalysts exhibit excellent activity and durability in the hydrolytic dehydrogenation of AB. Activated by the optimal [email protected] , the turnover frequency (TOF) and hydrogen generation rate (HGR) in the absence of any strong base are separately 136.6 min −1 and 30.3 × 10 3 mL min −1 g Ru −1 , and the apparent activation energy is 42.1 kJ mol −1 . Interestingly, the introduction of NaOH (2.0 M) can further significantly accelerate hydrogen release (TOF = 562.9 min −1 , HGR = 124.7 × 10 3 mL min −1 g Ru −1 ). Additionally, the kinetic isotope effect of 2.82 recommends that an O–H bond dissociation in water acts a dominant role in AB hydrolysis over [email protected] . This work develops a facile and environmentally friendly method for preparing supported metal-based nanocatalysts that can be effectively used in many reactions including AB hydrolysis.
研究领域:
材料化学
·
纳米催化
·
能源化学
·
绿色化学
·
氢能源
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Shi-Long Yang,Shi-Nuo Liu,Kang-Jian Du,Xiu-Cheng Zheng,Zhi-Kun Peng,Pu Liu
Simultaneously considering cost, safety and catalytic efficiency, the development of a cost-effective and high-performance catalyst is significant and challenging for controllable hydrogen release from ammonia borane (AB, NH 3 BH 3 ) hydrolysis. In this work, Ru ultrafine particles are evenly and firmly stabilized on wheat straw-derived porous carbon through a facile procedure. Specifically, attributed to the abundant co-doping of heteroatoms (namely, N and O) and suitable hierarchical porous structure of WSC-1.0 with large specific surface area (1000 m 2 g −1 ), which is prepared with a mass ratio of 1: 1 for K 2 CO 3 to the pre-carbonized biomass waste, as well as high dispersion (32.6%) of Ru ultrafine particles with an average size of 1.4 ± 0.3 nm, the optimal Ru/WSC-1.0 displays exceptional catalytic performance in the hydrolysis of AB. The corresponding turnover frequency (TOF) and specific reaction rate ( r B ) are 167.7 min −1 and 4.07 × 10 4 mL min −1 g Ru −1 , respectively, and the apparent activation energy is 40.94 kJ mol −1 . Upon adding NaOH (1.0 M), the hydrolysis rate can be remarkably accelerated (TOF = 401.4 min −1 , r B = 9.75 × 10 4 mL min −1 g Ru −1 ). The isotope experiments show that the scission of an O-H bond in H 2 O by oxidative addition is the decisive step in this reaction. Impressively, the effective “on-off” control for the hydrolytic dehydrogenation reaction over Ru/WSC-1.0 can be easily realized by introducing certain amounts of Zn(NO 3 ) 2 and EDTA-2Na, separately. Our work delivers a facile approach for efficient utilization of agricultural wastes and offers a robust and cost-effective catalyst for the controllable hydrogen evolution from AB hydrolysis.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Hailiang Chu,Nianpu Li,Xueying Qiu,Yu Wang,Shujun Qiu,Ju-Lan Zeng,Yongjin Zou,Fen Xu,Lixian Sun
In this work, poly( N -vinyl-2-pyrrolidone) (PVP)-stabilized ruthenium nanoparticles (NPs) supported on bamboo leaf-derived porous carbon (Ru/BC) has been synthesized via a one-step procedure. The structure and morphology of the as-synthesized samples were characterized by means of X-ray diffraction (XRD), X-ray photoelectron spectrometry (XPS), scanning electron microscope (SEM) and transmission electron microscope (TEM). As a catalyst for hydrogen generation from the hydrolysis of ammonia-borane (AB, NH 3 BH 3 ) at room temperature, Ru/BC stabilized with 1 mg of PVP exhibited high activity (TOF = 718 mol H2 ·mol Ru −1 ·min −1 ) and low activation energy ( E a = 22.8 kJ mol −1 ). In addition, the catalyst could be easily recovered and showed fairly good recyclability with 55.6% of the initial catalytic activity retained after ten experimental cycles, which confirmed that PVP could stabilize the Ru NPs and prevent their agglomeration on BC surface. Our results suggest that PVP-stabilized Ru/BC is a highly efficient catalyst for the hydrolysis of AB.
研究领域:
材料化学
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催化化学
·
纳米材料
·
能源化学
·
绿色化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Jialu Shen,Weifeng Chen,Guo Lv,Zihan Yang,Jiaying Yan,Xiang Liu,Zhongxu Dai
Recently, effective hydrogen (H 2 ) evolution upon hydrolysis of different hydrogen storage materials has received much attention. Herein, graphene quantum dots-transition metal nanoparticles (GQDs-TMNPs), with high dispersibility and activity, have been successfully applied in the hydrolysis of both NH 3 BH 3 (AB) and NaBH 4 for the first time. GQDs-RhNPs, GQDs-RuNPs, and GQDs-PtNPs are very effective in the hydrolysis of AB and the turnover frequencies (TOFs) can achieve to as high as 656, 384, and 281 mol H2 ·mol cat −1 min −1 , respectively. Moreover, the synergistic effect between GQDs and TMNPs is explored, and the mechanisms of catalytic hydrolysis of AB and NaBH 4 by GQDs-TMNPs are proposed. This work not only paves the way for the development of GQDs-TMNPs nanocatalysts for the different hydrogen storage materials, but also further advances the understanding of the synergistic effects between GQDs and TMNPs.
研究领域:
材料科学
·
催化化学
·
氢能储存
✓ 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
CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Xigang Du,Hongyu Liu,Mengfan Su,Yuping Tai,Bingli Pan,Ning Guo,Jun Zhang
Ru nanoparticles doped and supported by Mo oxide (Ru/Mo oxide NPs) were synthesized via an in situ co-precipitation strategy for hydrogen production via hydrolysis of ammonia borane (AB). The optimized Ru 0.9 Mo 0.1 catalyst composition exhibited a total turnover frequency (TOF) value of 514.8 mol H2 (mol Ru0.9Mo0.1 ) −1 min −1 at room temperature. Systematic characterization of the catalysts unveiled the dual role of Mo oxide in regulating the structure and catalytic performance of Ru NPs. This work provides a new approach for the design of Ru-based nanocatalysts toward hydrolysis of AB for H 2 harvest.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Qi Rong,Wenkai Huang,Fuhua Xu,Yanlan Wang,Changlong Wang,Xiang Liu
In spite of significant developments are accomplished in the exploration of H 2 and O 2 evolution upon water electrolysis/photolysis, this remains a challenge to design and develop ideal catalytic systems for this reaction and to isolate H 2 from H 2 -O 2 mixture with membranes. Herein, a series of ZIF-67-supported transition metal nanoparticles (TMNPs/ZIF-67), including Pt, Ir, Pd, Rh, Au and Ag, via immobilization of ultrafine TMNPs at the surface of ZIF-67, have been designed and developed for the selective H 2 generation from NH 3 BH 3 hydrolysis and O 2 evolution upon H 2 O 2 decomposition. In particular, the optimized nanocatalyst Pt/ZIF-67 presents the super-high catalytic property in the both H 2 evolution upon NH 3 BH 3 hydrolysis (689 mol(H 2 )·mol Pt -1 ·min −1 ) and O 2 evolution upon H 2 O 2 decomposition (979 mol(O 2 )·mol Pt -1 ·min −1) at 30 °C. Importantly, the selective “on–off” control for demand-based H 2 generation from NH 3 BH 3 hydrolysis was successfully realized by Zn 2+ /EDTA-2Na system. This highly efficient Pt/ZIF-67 proposed a new method for the promising potential application of ammonia borane and hydrogen peroxide as an economic and safe H 2 resp. O 2 carrier for fuel cell.
研究领域:
化学催化
·
燃料电池材料
·
纳米材料
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2018
·Vol. 10
·期 7
·1620-1626
·
IF 4.674
Wei Wang,Zhang-Hui Lu,Yan Luo,Aihua Zou,Qilu Yao,Xiangshu Chen
Graphical Dispersed Nanoparticles : Highly dispersed PdNi nanoparticles (NPs) have been successfully immobilized on mesoporous carbon nitride (MCN) through a facile co-reduction approach, which shows excellent catalytic performance for hydrogen release from an ammonia borane (AB) aqueous solution at room temperature. Highly dispersed Pd and PdNi nanoparticles (NPs) have been successfully immobilized on mesoporous carbon nitride (MCN) through a facile co-reduction approach. The resulting Pd/MCN catalyst shows excellent catalytic performance for hydrogen release from an ammonia borane (AB) aqueous solution with a turnover frequency (TOF) value of 125 mol H 2 mol metal −1 min −1 at room temperature, which is among the highest values for monometallic Pd-based catalysts reported to date. The catalytic performance of the Pd NPs can be further enhanced by alloying with Ni or Co atoms. Among all the synthesized Pd x Ni 100− x /MCN nanocomposites (NCs) with different Ni/Pd ratios, the Pd 74 Ni 26 /MCN catalyst exhibits the best catalytic performance with a TOF of 246.8 mol H 2 mol metal −1 min −1 . The high activity of Pd/MCN and Pd 74 Ni 26 /MCN are largely dependent on the features of the ultrafine metallic NPs immobilized by MCN, the interfacial interaction between the MCN matrix and metallic NPs, and the accessible open porous structure for mass transfer.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Environmental Progress & Sustainable Energy
·
2023
·Vol. 42
·期 6
·e14161
·
IF 2.8
Jie Cao,Fatao Zhang,Ting Xiao,Lihua Jiang,Weifeng Chen,Xinyu Tan
Utilizing the low-cost catalysts with excellent catalytic activities to replace the expensive ones for H 2 evolution still faces great challenges. It is significant to design the new catalysts with the synergistic effect to improve the activities and decrease the cost of the applications. Herein, the novel nanocatalyst of graphene quantum dots loaded bimetallic nanoparticles (Pt-Co/GQDs) has been synthesized for the H 2 evolution from hydrolysis of amine borane (AB) for the first time. The result indicates that the Pt-Co/GQDs nanocatalyst holds the better catalytic activities than Pt/GQDs, exhibiting the bimetallic synergies in the hydrolysis process. The synthesized catalyst has been characterized by various measurements, such as TEM, XPS, EDS, UV–Vis, and PL spectra. The effect of the catalyst on the hydrolysis of AB is investigated. It is demonstrated that the value of total turnover frequencies (TOFs) can arrive to 520 mol H 2 ·mol Pt −1 ·min −1 via the catalyst designing, which is very high in comparison with other reported catalysts. This work has developed an effective nanocatalyst with a lower cost which is never reported in the hydrolysis of AB, possessing both great significance and huge potential in the H 2 evolution by hydrolysis of the hydrogen storage materials.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
NANO
·
2022
·
IF 1.438
Jie Cao,Weimin Hu,Qiuyan Li,Guo Lv,Weifeng Chen,Xiang Liu
Utilization of nonprecious metals to replace precious metals in the catalytic hydrolysis of hydrogen storage materials causes wide attention. Herein, nonprecious bimetallic nanoparticles loaded on N-doped graphene quantum dots (Co-Ni/N-GQDs) have been synthesized and applied in the hydrolysis of NH 3 BH 3 for the first time. It is demonstrated that Co-Ni/N-GQDs exhibit the obvious bimetallic synergies in the hydrolysis of NH 3 BH 3 , and the total turnover frequency (TOF) value reaches 19.94 mol H2 ⋅ mol Cat − 1 ⋅ min − 1 via the optimized design. This work first explored the catalytic performance for the nonprecious bimetallic nanoparticles loaded on N-GQDs in the hydrolysis of NH 3 BH 3 , greatly facilitating the development of both nonprecious metals and N-GQDs in the hydrogen evolution.
研究领域:
材料科学
·
催化化学
·
氢能研究
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）