CHEMICAL ENGINEERING SCIENCE
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2023
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IF 4.7
Xiaoge Peng,Zhikang Bao,Shijie Zhang,Yuanan Li,Lei Ding,Huaijie Shi,Jia Liu,Xing Zhong,Xiaonian Li,Jianguo Wang
Assembling two desirable half-reactions of green oxidants hydrogen peroxide (H 2 O 2 ) and ozone (O 3 ) into efficient paired electrolysis is highly valuable in terms of efficiency and environmental-friendliness. However, rational design and construction of electrocatalysts with regulable active sites for the paired electrosynthesis of green oxidants of H 2 O 2 and O 3 remain a significant challenge. Herein, A new strategy was developed for tunning the active sites of pseudo-hexagonal centers (TT, Lewis acid sites) and orthogonal centers (T, Brønsted acid sites) in Mxene layered structure niobium pentoxide (Nb 2 O 5 ) with abundant oxygen vacancy (O V ) for the paired electrolysis of 2e - oxygen reduction reaction (ORR) and electrochemical ozone production (EOP). The TT-300 and T-400 electrocatalysts exhibited outstanding electrochemical activity of 2e - ORR (H 2 O 2 selectively of 92% at 0.4 V RHE ) and EOP (gaseous ozone FE of 13% at 50 mA cm −2 ), respectively. The excellent performance was mainly attributed to the TT-300 (Lewis acid sites) and T-400 (Brønsted acid sites) with abundant O V that improve the oxygen-containing intermediates formation of OOH* and deprotonation of water. In addition, the in-situ electro-degradation of organic compounds experiments indicated that the synergistic degradation of O 3 and H 2 O 2 possessed a faster kinetic constant compared with a single electrolysis system of O 3 and H 2 O 2 . The work provides meaningful insights into the rational design and construction of advanced solid acid electrocatalysts for efficient simultaneously electrocatalytic hydrogenation and oxidation to produce green oxidants of O 3 and H 2 O 2 .
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Siyu Ma,Zhihao Wang,Bowen Liu,Xiaolei Wang,Shichao Du,Zichen Song,Xinxin Bian,Manchen Hao,Ju Huang,Zhimin Chen,Zhiyu Ren
Pairing the hydrogen evolution reaction (HER) with the thermodynamics-friendly electrooxidation reaction (EOR) is a powerful way to maximize the energy/economic effectiveness, but still a challenge. Herein, the symbiotic Ni/MoN heterojunction arrays were constructed on foam (Ni/MoN/NF) by the nitridation-induced in situ reduction/conversion strategy. The fascinating interfacial electronic structure and surface reconstruction of Ni/MoN/NF heterojunction are responsible for the enhanced HMF-H 2 O paired electrolysis. Ni/MoN/NF only requires a low overpotential of 53 mV to reach the HER current density of 10 mA cm −2 , as well as the good durability; and NiOOH derived on the anode are electronically activated by MoN to achieving high-efficiency conversion from HMF to FDCA (∼100 % conversion, 97.5 % yield and 97.4 % Faradaic efficiency). For the HMF-H 2 O paired electrolysis, the assembled Ni/MoN/NF||Ni/MoN/NF electrolyzer only requires a low potential of 1.391 V to yield the current density of 10 mA cm −2 , ranking at the forefront in the reported coupling catalysts. Theoretical calculations manifest that the upshift of d -band center of the NiOOH/MoN heterojunction contributes to HMF chemisorption and activation, thereby enhancing its catalytic activity towards HMFEOR. Our study sheds light on the significance of designing the paired electrolysis with low voltage input for renewable energy applications.
研究领域:
材料科学
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能源化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Lixue Zhou,Daming Feng,Zhiqiang Li,Hui Li,Chunhua Ge,Xiangdong Zhang,Tianyi Ma
High-entropy materials offer unique advantages in catalysis due to lattice distortion, compositional complexity, and entropy-driven stability. In this study, we report a crystal phase-engineered high-entropy perovskite oxide, LaB 5 O 3 (B═Fe, Cu, Co, Cr, and Ni), which enables efficient bifunctional electrocatalysis. Structural transformation from orthorhombic to cubic symmetry modulates the spin states of B-site metals, particularly stabilizing the high-spin state of Fe 2 ⁺/Fe 3 ⁺, enhancing electron density and nitrate adsorption. This leads to a NH 3 Faradaic efficiency (FE) of 95.83% at −0.7 V vs. RHE for nitrate reduction (NO 3 RR), with minimal NO 2 ;− byproduct (FE < 2%). Concurrently, LaB 5 O 3 exhibits excellent sulfide oxidation reaction (SOR) activity, requiring only 0.484 V vs. RHE at 10 mA cm −2 —considerably lower than oxygen evolution reaction (OER) overpotential. Integrated into a paired electrolyzer, the system achieves simultaneous nitrate-to-ammonia conversion (max FE: 81.27%) and sulfide-to-sulfur transformation at a cell voltage of just 1.079 V. The superior performance arises from synergistic effects of high-entropy design, including enhanced oxygen vacancy formation, lattice strain, and ferroelectricity. This work demonstrates the potential of crystal phase engineering in high-entropy oxides for sustainable nitrogen fixation and sulfur recovery in water treatment applications.
研究领域:
材料科学
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环境催化
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电化学
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能源化学
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水处理技术
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无机功能材料
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可持续化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jiuli Chang,Lili Wang,Zhanqiang Hu,Songsong Zhi,Dapeng Wu,Kai Jiang,Zhiyong Gao
Selective ethylene glycol oxidation reaction (EGOR) to specific C2 species offers a promising approach to pair with cathodic hydrogen evolution reaction (HER) for electrochemical upcycling of waste polyethylene terephthalate (PET) plastic into high-value chemicals and H 2 . Efficient catalyst with tailored adsorptive interaction strength with intermediates is pivotal to fulfill such a scenario. Herein, a self-supported PdNi/NF electrode with deposition of PdNi hybrid onto nickel foam (NF) substrate was prepared by a gentle replacement reaction, which demonstrated high catalytic activity for EGOR toward glycolate with high faradaic efficiency (90 ± 2 %), decent yield (0.7 ± 0.01 mmol h −1 cm −2 ) and acceptable stability at a low applied potential of 0.8 V, which enabled electrosynthesis of glycolate via electrooxidation of PET hydrolysate. Meanwhile, a self-supported Cu, Co bimetallic phosphide onto NF substrate (CuCoP/NF) was prepared for HER catalysis, which featured a low overpotential of 117 mV at cathodic current density ( J ) of −100 mA cm −2 and decent durability. The further pairing of anodic EGOR and cathodic HER enabled electrolysis of PET hydrolysate to coproduce glycolate and H 2 at an energy-saving manner. This work provides a viable paradigm for coproduction of glycolate and H 2 from electrochemical upcycling of PET plastic, and presents essential instruction for reclamation of obsolete resource via sustainable and waste-to-treasure manner.
研究领域:
电化学
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催化
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高分子科学
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能量转换
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废物资源化
✓ 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）