Nano Energy
·
2025
·
IF 17.1
Zongnuo Sha,Cheng Hu,Shuchen Tu,Tong Li,Fang Chen,Hongwei Huang
Solar catalysis efficiency is severely subject to the insufficient charge separation and inactive surface sites. Building piezoelectric field is established to be effective for anisotropic photocharge separation, and introducing defects can enrich surface reactive sites. However, the relationship between piezoelectric field and surface defect or reaction kinetics remains unclear. Herein, we report piezo-activating oxygen vacancy (OVs) to regulate quantum well effect and p-band center for exceptional photocatalysis in polar BiOIO 3 single crystals. The introduction of piezoelectric field enhances the local charge asymmetry distribution induced by OVs, facilitating electron donating from bulk to surface I atom. Remarkably, the external strain collaborates with OVs to largely reduces the work function of its surface, and induces a larger up-shift of p-band center of I 5p orbitals in BiOIO 3 . It indicates a reduction in the occupancy of antibonding-orbital, facilitating the stabilization of O 2p antibonding states and formation of I-O ads bonds for strong O 2 /H 2 O adsorption. Thus, oxygen-vacant BiOIO 3 achieves a dramatically improved piezo-photocatalytic degradation efficiency towards various pollutants, outperforming the related piezo-photocatalysts in previous reports. This work reveals the mechanism of piezoelectric field on surface vacancy and surface electronic structure at the atomic level.
研究领域:
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yuci Xin,Yong Wu,Xingan Dong,Yuhan Li,Zhenxiang Cheng,Jianli Wang,Xiaolong Guo,Peng Yu
Amorphous electrocatalysts display several unique advantages in electricity-driven water splitting compared to their crystalline analogs, but understanding their structure–activity relationships remains a major challenge. Herein, we show that the d- and p-electronic states of amorphous Ni-Fe-B can be subtly manipulated by varying the Ni and Fe contents. The optimal Ni-Fe-B alloy exhibits a high performance in the oxygen evolution reaction (OER), as supported by its impressive stability (no clear degradation after 100 h) and considerably lower overpotential compared to those of its crystalline analogs. Based on theoretical calculations, different Ni and Fe contents can cause significant shifts in the d-band levels of Ni and Fe and the p-band level of B, thus altering the OER activity. Additionally, the energy difference between the d- and p-band centers (ΔE ad-p ) may be an effective index for use in reflecting the structure–activity relationship of an amorphous Ni-Fe-B alloy in the OER. An amorphous Ni-Fe-B alloy with a smaller ΔE ad-p displays a higher intrinsic activity. This study supplies a unique direction for use in constructing the structure–activity relationships of amorphous electrocatalysts by revealing the role of ΔE ad-p , which promotes fundamental research and the practical application of amorphous electrocatalysts.
研究领域:
材料科学
·
电催化
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Ning Sun,Yang Qin,Gongjin Xu,Yalei Fan,Bowen Zhang,Yu-Cheng Huang,Ying-Rui Lu,Xiangjiang Dong,Lei Lian,Zhichuan Zheng,Ruyue Wang,Qingyu Kong,Zhiwei Hu,Linjuan Zhang,Ming Lei,Kai Huang,Runze Yu
Atomic-scale modulation of crystalline ordering in heterogeneous catalysts offers a critical pathway to enhance reaction kinetics, yet fundamental understanding of how their dynamic structural evolution governs active-site stability remains elusive. Here, we decode these effects by precisely engineering crystallographic gradients from ordered to disordered states, within octahedral building blocks (isolated octahedra [MO 6 ] or dimer [M 2 O 9 ]) of perovskite oxides Ba 3 M x Ru 2-x O 9 (M = Fe, Co). This atomic-level control induces systematic shifts in d / p -band centers and optimizes charge distribution architectures within active regions. Crucially, the highly disordered Ba 3 FeRu 2 O 9 achieves exceptional stability via a self-sacrificial reduction of iron, which generates a built-in electric field (BEF). The BEF promotes optimal adsorption/desorption kinetics of OH*/H* intermediates for the hydrogen evolution reaction (HER). Consequently, Ba 3 FeRu 2 O 9 delivers benchmark alkaline HER performance, achieving an overpotential of just 24 mV at 10 mA cm −2 and demonstrating operational stability exceeding 600 h. Our results reveal that structural reorganization, enabled by atomic-level ordering modulation, is critical for establishing dynamic structure-performance frameworks to guide advanced catalyst design.
研究领域:
材料化学
·
电化学
·
催化化学
·
固态化学
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 51
·期 2
·541-552
·
IF 4.39
Dong Fang,Linlin Zhang,Yongjian Niu,Yuanyuan Wang,Qingxiao Su,Jiao Wang,Cheng Wang
SnO2 is one of the most promising catalysts for CO2 electroreduction. However, the intrinsic low electrical conductivity and weak CO2 adsorption and activation capability have rendered the reaction kinetically sluggish and inefficient. To surmount these hurdles, herein, W was incorporated into SnO2 nanosheets to modulate the electronic structures. Compared with pristine SnO2, the p-band centre of W-doped SnO2 was elevated towards the Fermi level, accompanied by the reduction in the band gap and work function. As a result, both the CO2 adsorption and the electron transfer process were promoted, thus lowering the activation energy barrier for CO2 reduction. Benefitting from these, a maximum faradaic efficiency of 87.8% was achieved for HCOOH at −0.9 V vs. the RHE. Meanwhile, the current density and energy efficiency approached 20.92 mA cm−2 and 60%, respectively. Such performances could sustain for 14 h without obvious fading and exceeded pristine SnO2 and most reported Sn-based catalysts. Tafel slope and reaction order analyses further suggested that the reaction proceeded following a stepwise electron–proton transfer pathway with the formation of CO2˙− as the rate determining step. This work demonstrated the effectiveness of electronic structure tuning in promoting the catalytic performances of p-block metal oxides and contributed to the development of efficient catalysts for sustainable energy conversion and carbon neutrality.
研究领域:
材料科学
·
电化学
·
催化
·
可持续能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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