FUEL
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2024
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IF 6.7
Yuyang Cao,Shilong Yang,Yuting Liu,Xingyu Liu,Yue Li,Xiucheng Zheng,Zhikun Peng,Pu Liu
At present, controllable producing hydrogen from the catalytic hydrolysis of ammonia borane (AB, NH 3 BH 3 ) is very meaningful and challenging. Therefore, developing an effective catalyst for the reaction, clarifying its catalytic mechanism, and realizing controllable hydrogen release are extremely indispensable. In this work, RuPd nanoalloys are evenly confined by the agricultural waste wheat straw-derived carbon (denoted as WSC) with a micropore-dominant porous structure and plentiful N/O doping. Attributing to the particular support effect of WSC and the interesting RuPd alloy effect, the as-prepared bimetallic catalysts provide encouraging catalytic performance in AB hydrolysis. Catalyzed by the optimal Ru 0.50 Pd 0.50 @WSC, the turnover frequency (TOF) and hydrogen evolution rate are 214.5 min −1 and 50800 mL min −1 g −1 , respectively, and the apparent activation energy is only 23.2 kJ mol −1 . Moreover, introducing proper NaOH (1.5 M) further accelerates hydrogen release (TOF = 502.8 min −1 , specific rate = 119100 mL min −1 g −1 ). The isotope experiments depict a kinetic isotope effect of 2.85, evidencing the vital role of the hydrogen–oxygen bond scission in this catalytic reaction. More importantly, benefitting from the difference in adsorption energy and strong coordination ability, the “on–off” control for the hydrolysis of AB over Ru 0.50 Pd 0.50 @WSC can be realized with the Zn 2+ /EDTA 2- system. This study provides an attractive metal alloy catalyst and some insights for the controllable hydrolysis of AB.
研究领域:
化学
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材料科学
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催化反应
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Qijing Zhang,Hongxia Yu,Siyi Wang,Haibo Li,Suyuan Zeng,Rui Li,Qingxia Yao,Qi Zhang,Ruru Chen,Lijian Meng,Konggang Qu
Overall water splitting (OWS) is the most potential method for large-scale hydrogen production, but the high-potential and sluggish oxygen evolution reaction (OER) greatly impedes its efficacy. Coupling the low-potential hydrazine oxidation reaction (HzOR) with the cathodic hydrogen evolution reaction (HER) has drawn widespread attention with energy-saving advantage and safe products, which necessitates the elaborate design of advanced bifunctional electrocatalysts. Herein, only using two complexes of Ru and Pd with 2,2′-bipyridine, the novel RuPd alloy/N-codoped carbon (RuPd/NC) composite was originally synthesize by direct mixing and pyrolysis, showing superior dual activity for HER and HzOR. Particularly, to deliver the current density of 10 mA cm −2 , RuPd/NC merely needs the potentials of −8 and −42 mV for alkaline HER and HzOR, far outperforming Pt/C and being most advanced among the previously studied counterparts. Moreover, the two-electrode overall hydrazine splitting (OHzS) needs ultrasmall voltages of 0.042 and 0.239 V to achieve 10 and 100 mA cm −2 , displaying great energy-saving feature. Moreover, the better activity for neutral HER, HzOR and OHzS on RuPd/NC was also found compared with Pt/C. The theoretical simulations uncover the water dissociation at Ru site with the greatly reduced energy barrier followed by the H desorption on the adjacent Pd site for HER, and the optimum activation energy on Ru site for HzOR, crediting to the synergistic regulation of alloying effect and metal-substrate interaction.
研究领域:
电催化
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材料化学
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能源科学
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纳米材料
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物理化学
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可持续能源技术
✓ 已验证
产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2025
·
IF 6.7
Hehe Qian,Tinghui Ma,Lili Shi,Shu Yan,Haisong Cui,Xueqing Luo,Fang Chen,Yuetan Su,Zhongbiao Wu,Xiaole Weng
Electrocatalytic hydrodechlorination (EHDC) is a promising strategy for remediating chlorinated organic pollutants by utilizing reactive hydrogen (H*) to cleave C–Cl bonds. Addressing the challenge of simultaneously optimizing H* generation and targeted pollutant adsorption/activation, this work introduces synergistic surface engineering of RuPd alloy nanocatalysts. Compositionally controlled RuPd nanoparticles (RuPd2, Ru2Pd3, and Ru2Pd) were synthesized via seed-mediated growth, yielding uniform sub-3.5 nm nanoparticles with homogeneous elemental distribution. The optimal RuPd2 electrocatalysts achieved 97.1% 2-chlorophenol conversion within 6 h at −0.85 V vs Ag/AgCl, exhibiting a mass activity of 28.3 min–1 g–1Pd, representing a 5.6-fold enhancement over monometallic Pd. Moreover, RuPd2 demonstrated enhanced durability, maintaining performance with less than 5% efficiency loss over 10 cycles. This enhanced EHDC performance originated from dual synergistic effects. Electron transfer from Ru to Pd facilitated H* generation kinetics, evidenced by a near-optimal ΔGH* (−0.25 eV) at Pd–Pd–Pd hollow sites, while Ru-rich surface domains significantly strengthened 2-chlorophenol adsorption and elongated the C–Cl bond to facilitate dechlorination. These spatially separated synergistic sites collectively achieve higher EHDC efficiency, establishing a unified catalyst design strategy that effectively orchestrates coupled surface processes, and provides a significant advance for efficient EHDC technology with broad environmental remediation implications.
研究领域:
环境催化
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纳米材料化学
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污染物降解
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电化学
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表面科学
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能源与环境工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）