Abstract
Ambient sunlight-driven CO
2
methanation cannot be realized due to the temperature being less than 80 °C upon irradiation with dispersed solar energy. In this work, a selective light ...absorber was used to construct a photothermal system to generate a high temperature (up to 288 °C) under weak solar irradiation (1 kW m
−2
), and this temperature is three times higher than that in traditional photothermal catalysis systems. Moreover, ultrathin amorphous Y
2
O
3
nanosheets with confined single nickel atoms (SA Ni/Y
2
O
3
) were synthesized, and they exhibited superior CO
2
methanation activity. As a result, 80% CO
2
conversion efficiency and a CH
4
production rate of 7.5 L m
−2
h
−1
were achieved through SA Ni/Y
2
O
3
under solar irradiation (from 0.52 to 0.7 kW m
−2
) when assisted by a selective light absorber, demonstrating that this system can serve as a platform for directly harnessing dispersed solar energy to convert CO
2
to valuable chemicals.
Solar-heating catalysis has the potential to realize zero artificial energy consumption, which is restricted by the low ambient solar heating temperatures of photothermal materials. Here, we propose ...the concept of using heterostructures of black photothermal materials (such as Bi
Te
) and infrared insulating materials (Cu) to elevate solar heating temperatures. Consequently, the heterostructure of Bi
Te
and Cu (Bi
Te
/Cu) increases the 1 sun-heating temperature of Bi
Te
from 93 °C to 317 °C by achieving the synergy of 89% solar absorption and 5% infrared radiation. This strategy is applicable for various black photothermal materials to raise the 1 sun-heating temperatures of Ti
O
, Cu
Se, and Cu
S to 295 °C, 271 °C, and 248 °C, respectively. The Bi
Te
/Cu-based device is able to heat CuO
/ZnO/Al
O
nanosheets to 305 °C under 1 sun irradiation, and this system shows a 1 sun-driven hydrogen production rate of 310 mmol g
h
from methanol and water, at least 6 times greater than that of all solar-driven systems to date, with 30.1% solar-to-hydrogen efficiency and 20-day operating stability. Furthermore, this system is enlarged to 6 m
to generate 23.27 m
/day of hydrogen under outdoor sunlight irradiation in the spring, revealing its potential for industrial manufacture.
Cu-based nanocatalysts are the cornerstone of various industrial catalytic processes. Synergistically strengthening the catalytic stability and activity of Cu-based nanocatalysts is an ongoing ...challenge. Herein, the high-entropy principle is applied to modify the structure of Cu-based nanocatalysts, and a PVP templated method is invented for generally synthesizing six-eleven dissimilar elements as high-entropy two-dimensional (2D) materials. Taking 2D Cu
Zn
Al
Ce
Zr
O
as an example, the high-entropy structure not only enhances the sintering resistance from 400 °C to 800 °C but also improves its CO
hydrogenation activity to a pure CO production rate of 417.2 mmol g
h
at 500 °C, 4 times higher than that of reported advanced catalysts. When 2D Cu
Zn
Al
Ce
Zr
O
are applied to the photothermal CO
hydrogenation, it exhibits a record photochemical energy conversion efficiency of 36.2%, with a CO generation rate of 248.5 mmol g
h
and 571 L of CO yield under ambient sunlight irradiation. The high-entropy 2D materials provide a new route to simultaneously achieve catalytic stability and activity, greatly expanding the application boundaries of photothermal catalysis.
Methanol dehydrogenation is an efficient way to produce syngas with high quality. The current efficiency of sunlight-driven methanol dehydrogenation is poor, which is limited by the lack of excellent ...catalysts and effective methods to convert sunlight into chemicals. Here, we show that atomically substitutional Pt-doped in CeO2 nanosheets (Pts-CeO2) exhibit excellent methanol dehydrogenation activity with 500-hr level catalytic stability, 11 times higher than that of Pt nanoparticles/CeO2. Further, we introduce a photothermal conversion device to heat Pts-CeO2 up to 299°C under 1 sun irradiation owning to efficient full sunlight absorption and low heat dissipation, thus achieving an extraordinarily high methanol dehydrogenation performance with a 481.1 mmol g−1 h−1 of H2 production rate and a high solar-to-hydrogen (STH) efficiency of 32.9%. Our method represents another progress for ambient sunlight-driven stable and active methanol dehydrogenation technology.
Display omitted
•Atomically substitutional Pt-doped CeO2 is active and robust for CH3OH dehydrogenation•The photothermal conversion device can heat Pts-CeO2 to 299°C under 1 sun irradiation•The joint system achieves a one sun irradiated H2 production rate of 481.1 mmol g−1 h−1•This system delivers a high solar-to-H2 efficiency of 32.9% under one sun irradiation
Catalysis; Chemical Reaction Engineering; Chemistry
In this work, we present a novel artificial photosynthetic paradigm with square meter (m2) level scalable production by integrating photovoltaic electrolytic water splitting device and solar heating ...CO2 hydrogenation device, successfully achieving the synergy of 1 sun driven 19.4% solar to chemical energy efficiency (STC) for CO production (2.7 times higher than that of large-sized artificial photosynthetic systems) with a low cost (equivalent to 1/7 of reported artificial photosynthetic systems). Furthermore, the outdoor artificial photosynthetic demonstration with 1.268 m2 of scale exhibits the CO generation amount of 258.4 L per day, the STC of ~15.5% for CO production in winter, which could recover the cost within 833 sunny days of operation by selling CO.
Converting carbon dioxide (CO2) into value-added fuels or chemicals through photothermal catalytic CO2 hydrogenation is a promising approach to alleviate the energy shortage and global warming. ...Understanding the nanostructured material strategies in the photothermal catalytic CO2 hydrogenation process is vital for designing photothermal devices and catalysts and maximizing the photothermal CO2 hydrogenation performance. In this Perspective, we first describe several essential nanomaterial design concepts to enhance sunlight absorption and utilization in photothermal CO2 hydrogenation. Subsequently, we review the latest progress in photothermal CO2 hydrogenation into C1 (e.g., CO, CH4, and CH3OH) and multicarbon hydrocarbon (C2+) products. Finally, the relevant challenges and opportunities in this exciting research realm are discussed. This perspective provides a comprehensive understanding for the light–heat synergy over nanomaterials and instruction for rational photothermal catalyst design for CO2 utilization.
Photocatalytic selective catalytic reduction of nitrogen oxides (NOx SCR) is a green and effective method to eliminate NOx. But the natural sunlight-driven NOx SCR is not realized due to the low ...temperature under sparse sunlight irradiation and the lack of highly active catalysts. To solve those problems, we selected a commercial AlNx film which can heat the catalysts to 270 °C just under one standard solar irradiation because of its full sunlight absorption and low radiation characteristics, enabling to onset NOx SCR. Further, a polyvinyl alcohol assisted graphene oxides templated method was developed to synthesize the W doped Fe2O3 nanosheets on a large scale, which can be used as efficient NOx SCR catalysts with high N2 selectivity, excellent SO2 and H2O resistances. As a result, the AlNx assisted W doped Fe2O3 nanosheets showed 92% and 90% NO conversion rate under one solar irradiation and outdoor sunlight irradiation respectively without second energy input, first time of realizing natural sunlight-driven photothermal NOx SCR. This strategy demonstrates a great potential on second energy free industrialized NOx SCR.
We found that a commercial AlNx film can convert 1 kW m−2 of sunlight as more than 270 °C high temprature due to its full sunlight absorption and low heat emission. As a result, the AlNx assisted W doped Fe2O3 nanosheets showed 92% NOx SCR efficiency under 1 kW m−2 of sunlight irradiation without second energy input. Display omitted
•AlNx film can convert 1 kW m−2 of sunlight as more than 270 °C high temperature.•W doped Fe2O3 nanosheets with high surface area of 310 m2 g−1 is synthesized at gram scale.•The NOx SCR efficiency of W doped Fe2O3 nanosheets is 28.3 times higher than that of normal W doped Fe2O3 structures.•One solar-driven photothermal AlNx assisted W doped Fe2O3 nanosheets shows 92% NOx SCR efficiency.•Natural sunlight-driven photothermal NOx SCR is realized by AlNx assisted W doped Fe2O3 nanosheets.
Sunlight driven formic acid decomposition has great potential to supply high-purity H2 without consuming fossil fuel-derived energy. However, a trace amount of CO invariably exists in the obtained H2 ...and the H2 production rate is always lower than 278 mmol g−1 h−1. Here, we found that high quality MoS2 grown on graphene decorated on Ni foam (Ni/G/MoS2) was active and stable for H2 production from thermocatalytic formic acid decomposition without CO presentation and first principles calculation confirmed that the perfect surface terminating sulfur of MoS2 changed the reaction path of intermediates, thus inhibiting the production of CO. Furthermore, a reaction device constructed with Cu2Se can heat catalysts to 120 and 260 °C under 0.25 kW m−2 and 1 kW m−2 (1 Sun) of irradiation, respectively. By using the system of the Cu2Se based reaction device and Ni/G/MoS2, a CO free H2 production rate of 982 mmol g−1 h−1 was achieved under 0.6 Sun of irradiation, 3.5 times higher than the previous record of photocatalytic formic acid decomposition. Therefore, this work provides a new viewpoint for large scale CO free H2 production in a sustainable and green way.
Sunlight driven formic acid decomposition has great potential to supply high-purity H
2
without consuming fossil fuel-derived energy. However, a trace amount of CO invariably exists in the obtained H
...2
and the H
2
production rate is always lower than 278 mmol g
−1
h
−1
. Here, we found that high quality MoS
2
grown on graphene decorated on Ni foam (Ni/G/MoS
2
) was active and stable for H
2
production from thermocatalytic formic acid decomposition without CO presentation and first principles calculation confirmed that the perfect surface terminating sulfur of MoS
2
changed the reaction path of intermediates, thus inhibiting the production of CO. Furthermore, a reaction device constructed with Cu
2
Se can heat catalysts to 120 and 260 °C under 0.25 kW m
−2
and 1 kW m
−2
(1 Sun) of irradiation, respectively. By using the system of the Cu
2
Se based reaction device and Ni/G/MoS
2
, a CO free H
2
production rate of 982 mmol g
−1
h
−1
was achieved under 0.6 Sun of irradiation, 3.5 times higher than the previous record of photocatalytic formic acid decomposition. Therefore, this work provides a new viewpoint for large scale CO free H
2
production in a sustainable and green way.
Using a combination of Ni/G/MoS
2
and a Cu
2
Se based reaction device, a CO free H
2
production rate of 982 mmol g
−1
h
−1
was achieved under 0.6 Sun of irradiation, 3.5 times higher than the previous record of photocatalytic formic acid decomposition.
Sunlight driven formic acid decomposition has great potential to supply high-purity H
2
without consuming fossil fuel-derived energy. However, a trace amount of CO invariably exists in the obtained H
...2
and the H
2
production rate is always lower than 278 mmol g
−1
h
−1
. Here, we found that high quality MoS
2
grown on graphene decorated on Ni foam (Ni/G/MoS
2
) was active and stable for H
2
production from thermocatalytic formic acid decomposition without CO presentation and first principles calculation confirmed that the perfect surface terminating sulfur of MoS
2
changed the reaction path of intermediates, thus inhibiting the production of CO. Furthermore, a reaction device constructed with Cu
2
Se can heat catalysts to 120 and 260 °C under 0.25 kW m
−2
and 1 kW m
−2
(1 Sun) of irradiation, respectively. By using the system of the Cu
2
Se based reaction device and Ni/G/MoS
2
, a CO free H
2
production rate of 982 mmol g
−1
h
−1
was achieved under 0.6 Sun of irradiation, 3.5 times higher than the previous record of photocatalytic formic acid decomposition. Therefore, this work provides a new viewpoint for large scale CO free H
2
production in a sustainable and green way.
PDF
