
氫能規模化應用的核心瓶頸在于安全高效的儲運技術。固態儲氫材料中,氫化鋁(AlH3)雖具有10.1wt%的超高理論容量,卻因本征熱力學穩定性過強,脫氫溫度高達150-200°C,不得不依賴外部電熱驅動。利用太陽能介入雖可擺脫外源電能束縛,然現有光熱路徑需歷經“光→熱→化學"的多級能量轉換,梯級損耗顯著;而紫外光催化路徑則受限于紫外波段僅占太陽光譜的4%,光子利用效率極低。因此,如何在寬光譜范圍內實現高效的光子-化學能直接轉化,突破AlH3的熱力學壁壘,便成為該方向亟待攻克的核心科學問題。
針對上述難題,安徽大學梁飛教授團隊創新性地提出了基于可見光驅動的非熱力學光催化調控策略,通過系統的實驗表征與理論計算,揭示了原位生成的Al/MOF異質結構中等離激元熱電子注入對界面電荷轉移的調控機制,并結合AlH3在光催化劑表面的化學吸附行為,實現了室溫超低光強下脫氫速率與儲氫釋放容量的雙重突破。這一發現為高能量密度固態儲氫體系的光催化脫氫提供了一種新的高效范式。
Figure 1. Schematic illustration of this study. Visible-light-driven photocatalytic dehydrogenation mechanism of AlH3.
排除干擾,直擊真相
在展示相關數據前,研究團隊首先解答了一個嚴謹的科學問題:MOF作為多孔材料,會不會因為物理吸附氫氣而造成“假陽性"或儲量流失?
Supplementary Figure 3的等溫吸脫附曲線給出了答案:在25°C、1 MPa壓力下,MOF的氫氣吸附量僅為0.056 wt.%,且在常壓(0.1 MPa)下幾乎不吸收氫氣。這一硬核數據排除了多孔材料物理吸氫的干擾,證實了MOF在復合體系中僅作為高效光催化劑存在,確保了后續實驗數據的絕對純凈與可靠。
Supplementary Figure 3. Hydrogen adsorption-desorption isotherm measurement of MOF at 25°C.
超低光強下的倍增奇跡
效率提升:在極低光強(0.37 W cm-2)的可見光照射下,最佳復合體系AlH3-MOF (1%) 的脫氫速率穩定在30.8 µmol g-1 min-1,較室溫暗環境(1.5 µmol g-1 min-1)足足提升了20.5倍。
超越純熱驅動:在無主動水冷、近環境溫度(55°C)下,光驅動180 min內的脫氫量達到4.7wt.%。對比同等溫度下的純熱驅動脫氫,光驅動的產氫量整整是熱驅動的2.1倍。
Figure 4. Visible-light-driven photocatalytic dehydrogenation performance and characterization of AlH3-MOF.
(a) Visible-light-driven hydrogen release profiles of AlH3-MOF and ball-milled AlH3 under visible light irradiation (0.56 W cm-2) at room temperature (with error bars representing the standard deviation: n = 3).
(b) Visible-light-driven hydrogen release profiles of AlH3-MOF (1%) under different light intensities at room temperature (with error bars representing the standard deviation: n = 3).
(c) Hydrogen release rates of AlH3-MOF (1%) at room temperature under (i) visible light irradiation (0.37 W cm-2) and (ii) dark conditions.
Supplementary Figure 14. Visible-light-driven (0.37 W/cm2) hydrogen release without active water-cooling and isothermal hydrogen release profile at 55 °C of AlH3-MOF (1%), respectively.
底層熱力學的“逆轉魔法"
化“吸熱"為“放熱":未受光激發的純AlH3脫氫路徑,其自由能變化(ΔG)為 + 0.56 eV,是一個熱力學上極度不利的吸熱過程。而耦合光催化劑后,界面電子的重新分布使得該路徑的ΔG降低為-0.09 eV,變為了自發的放熱反應。
打通決速步:在最艱難的脫氫決速步(AlH2 → AlH)中,光生載流子的精準介入使反應能壘大幅降低了39%(從1.73 eV驟降至1.05 eV)。

Figure 6. Density functional theory calculations of AlH3-Al/MOF. Side view of optimized structures
(a) before and (b) after adsorption of AlH3 cluster on Al/MOF surface.(c) Side view of the electron density difference map of AlH3-Al/MOF.
(d) H-1s PDOS of AlH3, Al/MOF, and AlH3-Al/MOF. (e) Free energy profiles for AlH3 complexation and stepwise dehydrogenation on Al/MOF surface.
(f) Al-H bond lengths of AlH3 after adsorption on Al/MOF surface.
國儀量子H-Sorb 4600PCT Pro高壓儲氫吸附儀
高壓儲氫吸附儀可以實現材料在不同溫度及不同高壓環境下對氫氣的吸放氫行為檢測,可有效表征材料吸放氫溫度和壓力、吸放氫量、吸放氫速率等儲氫材料吸放氫熱/動力學關鍵性能。

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全自動吸脫附變溫測試(PCT、Kinetics、Cycle)
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10.Structural and Phase Evolution in the Mg-Al System Leading to Lower Hydrogen Desorption Temperature. Hydrogen (2025)
11.Interpretable machine learning framework for hydrogen storage capacity prediction in Ti-Zr-Mn-Cr-V high-entropy alloys: Influenced by valence electron average. Journal of Energy Storage (2026)
12.Dual-strategy regulation for enhancing hydrogen storage performance of non-activated Mg8Ni-TiO2/MnO2 composites. Journal of Energy Chemistry (2025)
13.Nanoscale effect of spontaneous combustion of sulfur corrosion products: Oxygen adsorption and activation mechanism dominated by mesopores. Fuel (2026)
14.Pore structure reconfiguration and microscale fluid response in bituminous coal under CO2 and flue gas-enhanced coalbed methane recovery. Fuel (2026)
15.Experimental and theoretical investigation on hydrogen storage performance of titanium decorated hexagonal boron nitride. Applied Surface Science (2026)
16.Cu-based methanol steam reforming catalyst supported by heat conduction enhanced GO+UiO-66 composite MOF material for long-term stable hydrogen production. International Journal of Hydrogen Energy (2025)