3.1. Effect of Joint Application of Sewage Sludge and Fertilizers on the Growth of Rice and Wheat
The effect of joint application of SSL with chemical fertilizer (CF) at different growth stages (30, 60, 90 DAT/DAS and harvest stage) of rice and wheat crop is presented in
Table 1 and
Table 2. The greatest plant height was measured in treatment T
3, i.e., the combination of 30 Mg ha
−1 SSL + 100% RDF (104.22 cm) followed by T
2, i.e., 20 Mg ha
−1 SSL + 100% RDF (102.41 cm) at the harvest stage of III-rice and these treatments having significantly increased height compared to 100% RDF. However, treatment T
2 i.e., 20 Mg ha
−1 SSL + 100% RDF and T
3 i.e., 30 Mg ha
−1 SSL + 100% RDF were found to be statistically similar with respect to plant height at the harvest stage. A similar trend was noticed in III-wheat. During 2018–2019, the maximum plant height for IV-rice (102.32) and IV-wheat (103.80) at harvest stage was recorded in treatments T
3 (30 Mg ha
−1 SSL + 100% RDF), significantly greater than T
1 (100% RDF). However, T
3 (30 Mg ha
−1 SSL + 100% RDF) was statistically at par with treatment T
2 (20 Mg ha
−1 SSL + 100% RDF) in IV-rice and IV-wheat. In IV-wheat crop, application of 20 Mg ha
−1 SSL + 100% RDF (T
2) and 30 Mg ha
−1 SSL + 100% RDF (T
3) significantly increased plant height over 100% RDF (
Table 1 and
Table 2).
There was a significant reduction in plant height in T4 (50% RDF + 20 Mg ha−1 SSL) and T5 (60% RDF + 20 Mg ha−1 SSL), whereas T6 (70% RDF + 20 Mg ha−1 SSL), T7 (50% RDF + 30 Mg ha−1 SSL), T8 (60% RDF + 30 Mg ha−1 SSL) and T9 (70% RDF + 30 Mg ha−1 SSL) were at par with T1 (100% RDF). The plant heights in treatment T2 (100% RDF + 20 Mg ha−1 SSL) and T3 (100% RDF + 30 Mg ha−1 SSL) at harvest were 13.62 and 15.63% higher than T1 (100% RDF) in III-rice crop, and in IV-rice the same treatment had respective increases by 10.70 and 14.08% over T1 (100% RDF).
In the case of III-wheat, the respective increases in T
2 (100% RDF + 20 Mg ha
−1 SSL) and T
3 (100% RDF + 30 Mg ha
−1 SSL) were 11.82 and 15.09%, and for IV-wheat, 8.94 and 11.90% over T
1 (100% RDF). It was observed that at all the growth stages (30, 60 and 90 DAT/DAS), T
3 (30 Mg ha
−1 SSL + 100% RDF) and T
2 (20 Mg ha
−1 SSL + 100% RDF) showed the highest plant heights in rice and wheat crops (
Table 1 and
Table 2).
It is well-known that applying SSL with CF to croplands can enhance plant height. According to Latare et al. [
21] combining SSL with chemical fertilizers may improve soil fertility and increase the availability of nitrogen and trace elements to plants, thus indirectly enhanced plant development. The addition of SSL with CF enhances the direct availability of N and P from chemical fertilizers, and indirect or slow-release from SSL, which results in increased leaf area and higher dry matter accumulation [
42,
43]. Thus, the improvement of soil fertility associated with the application of SSL and CF would have supported improved rice and wheat plant growth. Similarly, Zhang et al. [
44] revealed a significant increase in rice plant height by greater soil fertility and nutrient status after applying SSL amendments. Our findings also resemble the work of Rehman and Qayyum [
45], who reported a significant influence of SSL compost on crop productivity and biomass accumulation in rice and wheat crops.
3.2. Leaf Greenness (SPAD) at Different Growth Stages of Rice and Wheat
The data presented in
Figure 3 show a significant increase of leaf greenness (chlorophyll content) in rice and wheat due to the joint application of SSL and CF in both years.
Maximum leaf greenness was measured in T3 (100% RDF + 30 Mg ha−1 SSL) followed by T2 (100% RDF + 20 Mg ha−1 SSL), and the minimum was in T0 (without SSL and CF). Treatment T3 (100% RDF + 30 Mg ha−1 SSL) and T2 (100% RDF + 20 Mg ha−1 SSL) had significantly increased leaf greenness over T1 (100% RDF) in III-rice, whereas these treatments were statistically similar with 100% RDF (T1) in III-Wheat.
However, the treatments from T4 toT9 showed a non-significant difference of T1 in terms of leaf greenness in III-rice and III-wheat in the year 2017–2018. Similarly, the treatments T2 (100% RDF + 20 Mg ha−1 SSL) and T3 (100% RDF + 30 Mg ha−1 SSL) were found statistically at par with each other in III-rice and III-wheat. During 2018–2019, the leaf greenness ranged from 24.84 to 44.01 and 25.13 to 43.27 SPAD in IV-Rice and IV-Wheat, respectively. The maximum leaf greenness in IV-Rice and IV-wheat, during both years was seen in T3, i.e., the combination of 30 Mg ha−1 SSL + 100% RDF at 30 DAT/DAS.
Although, it was noticed that the T
3 (100% RDF + 30 Mg ha
−1 SSL), treatment was statistically at par with T
1 (100% RDF), T
2 (100% RDF + 20 Mg ha
−1 SSL), T
6 (70% RDF + 20 Mg ha
−1 SSL), T
8 (60% RDF + 30 Mg ha
−1 SSL), and T
9 (100% RDF + 30 Mg ha
−1 SSL), it was significantly superior over the rest of the treatments in terms of leaf greenness in IV-rice and IV-wheat at 30 DAT during the year 2018–2019. An almost similar trend was observed with the leaf greenness recorded at 60 and 90 DAT/DAS. AT 60 DAT/DAS, a slight increase in plant leaf greenness was noticed compared to observations at 30 DAT/DAS, whereas at 90 DAT, a decrease was noticed compared to 30 and 60 DAT/DAS. Chlorophyll content (SPAD) directly influences the photosynthetic rate of plants. The increase in assimilatory pigments content in leaves was observed when crops were grown in SSL-amended soil. Romani and Beltarre [
46] found that repeated 7 years of treatment with SSL (3.7 Mg ha
−1) resulted in a significant increase in chlorophyll content (SPAD index). Latare et al. [
43] reported that at 30 days after transplanting and sowing (DAT/DAS) in rice and wheat, leaf greenness index did not increase but increased significantly at 60 and 90 DAT/DAS. This might be because Fe, Mg, and Mn contents in the SSL, are liberated after decomposition of SSL and remain directly associated with chlorophyll synthesis [
47,
48].
3.3. Effect of Sewage Sludge and Fertilizers on Yield Attributes of Rice and Wheat
The panicle/ear length (cm) ranged between 18.26–37.61 and 12.99–35.95 with mean values of 29.49 and 27.15 in III-Rice and IV-rice, respectively whereas the corresponding value in III-wheat and IV-wheat varied between 6.09–15.54 and 5.90–15.16 with a mean value of 11.89 and 11.28 (
Table 3). It was observed that for the rice crop, the significantly highest length of the panicle (37.61 and 35.95 cm) was recorded with T
3 (100% RDF + 30 Mg ha
−1 SSL) followed by T
2 (34.61 and 32.87 cm) during both years, respectively. An almost similar trend was noticed during both years of wheat experimentation. In III-Rice, a significant increase was recorded with T
2 (18.16%) and T
3 (28.41%) concerning panicle length. Similarly, the ear length of the wheat crop (III and IV) increased significantly in T
3 (29.50 and 20.03%) over 100% RDF (
Table 3). The result show that the application of SSL with CF increased ear/panicle length. This is due to the role of N in flowering, fruiting, and crop maturation, as well as seed formation. Latare et al. and Jamil et al. [
21,
49] reported an increase in spike length of wheat with different doses of SSL compared to the non-treated plot. A similar trend was observed in the wheat crop [
50]. Zhang et al. [
51] reinforced the results, finding that an adequate supply of organic wastes along with NPK fertilizer improves the yield attribute. Thus, combined application of SSL with chemical fertilizer in different levels appears beneficial with respect to yield attributes without showing any toxic effects on plants. The number of grains per panicle/ear (
Table 3) varied from 54.44 to 154 and 15.36 to 41.02 in III-rice and III-wheat (2017–2018), respectively. Application of 30 Mg ha
−1 SSL + 100% RDF resulted in the highest number of grains per panicle i.e., 154.41 and 41.02 in III-rice and III-wheat, respectively.
During 2018–2019, the maximum grains per panicle/ear for IV-rice (146.147) and IV-wheat (39.64) were measured in treatments T
3 (30 Mg ha
−1 SSL + 100% RDF). This was significantly superior to T
1 in IV-rice but statistically similar in IV-wheat (
Table 3). A significant reduction was noticed in grains per panicle in T
4 (50% RDF + 20 Mg ha
−1 SSL) and T
5 (60% RDF + 20 Mg ha
−1 SSL), whereas T
6 (70% RDF + 20 Mg ha
−1 SSL), T
7 (50% RDF + 30 Mg ha
−1 SSL), T
8 (60% RDF + 30 Mg ha
−1 SSL), and T
9 (70% RDF + 30 Mg ha
−1 SSL) were at par with T
1 (100% RDF) in IV-rice. While, IV-wheat showed a marked reduction in T
4 (50% RDF + 20 Mg ha
−1 SSL) and T
5 (60% RDF + 20 Mg ha
−1 SSL), T
6 (70% RDF + 20 Mg ha
−1 SSL), T
7 (60% RDF + 30 Mg ha
−1 SSL), T
8 (70% RDF + 30 Mg ha
−1 SSL), and T
9 (70% RDF + 30 Mg ha
−1 SSL) were statistically at par with respect to grains per panicle. T
2 (RDF 100% + SSL 20 Mg ha
−1) was 22.06% higher than T
1 (RDF 100%) in the III-rice crop, and in the case of IV-rice, the same treatment showed a 12.04% increase over T
1 (RDF 100%).
In the case of III-wheat, T
2 was 16.81% greater than T
1 (100% RDF), whereas this increase was only 4.93% in the IV-wheat crop. Tamrabet et al. [
52] found an increased number of grains spike
−1 of wheat after treatment with 20, 30, and 40 Mg ha
−1 SSL. Moreover, SSL seemed to be more beneficial l the crop than inorganic fertilizer. The SSL treatment statistically improved spike fertility and plant biomass at the heading and maturity stage. By applying SSL and fertilizer, the yield of both crops was significantly improved significantly in all the treatments compared to no fertilizer (
Figure 4).
In both years, in rice and wheat crops, a significantly higher grain yield was documented in T3, with the combination of 30 Mg ha−1 SSL + 100% RDF, followed by T2 with 20 Mg ha−1 SSL + 100% RDF, compared to other treatments, whereas the lowest yield was recorded in WF (T0).
There was no significant difference within the rest of the treatments except T4 (50% RDF + 20 Mg ha−1 SSL) and T5 (60% RDF + 20 Mg ha−1 SSL) compared to only 100% RDF (T1) in IV-rice and IV-Wheat. The grain yield in treatment T2 (100% RDF + 20 Mg ha−1 SSL) and T3 (100% RDF + 30 Mg ha−1 SSL) of III-rice was higher by 7.75% and 11.42%, respectively, compared to treatment T1 where 100% RDF was applied. In the case of IV-rice, the grain yield of treatments T2 (100% RDF + 20 Mg ha−1 SSL) and T3 (100% RDF + 30 Mg ha−1 SSL) was higher by 2.44% and 4.83%, respectively, than T1 (100% RDF). With III-wheat, the grain yield of treatment T2 (20 Mg ha−1 SSL + 100% RDF) and T3 (30 Mg ha−1 SSL + 100% RDF) showed a respective increase of 15.55% and 22.75% over T1 (100% RDF), whereas, in the case of IV-wheat, treatment T2 (20 Mg ha−1 SSL + 100% RDF) and T3 (30 Mg ha−1 SSL + 100% RDF) showed only 9.12% and 15.20% yield increment over T1 (100% RDF).
During 2017–2018, in III-rice, application of 100% RDF resulted in statistically similar grain yield in all other treatments except T
0 (WF). However, the yield of treatment T
1, i.e., 100% RDF, was at par with 20 Mg ha
−1 SSL when applied with reduced doses of CF (T
4, T
5 and T
6), and also with 30 Mg ha
−1 SSL with a reduced dose of CF (T
7, T
8 and T
9). This provides the option of reducing the dose of RDF up to 50% when applied with SSL. A similar trend was observed for the grain yield of III–wheat. During 2018–2019, grain yield of IV-Rice in T
1 (100% RDF) was statistically similar to T
2 (20 Mg ha
−1 SSL + 100% RDF), T
3 (30 Mg ha
−1 SSL + 100% RDF), T
6 (20 Mg ha
−1 SSL + 70% RDF), T
7 (30 Mg ha
−1 SSL + 50% RDF), T
8 (30 Mg ha
−1 SSL + 60% RDF) and T
9 (30 Mg ha
−1 SSL + 70% RDF). However, a significant reduction in grain yield was noticed in T
4 (20 Mg ha
−1 SSL + 50% RDF) and T
5 (20 Mg ha
−1 SSL + 60% RDF). An almost similar yield trend was observed for IV wheat. It is evident that providing only 50% RDF with 20 Mg ha
−1 SSL resulted in yields similar to 100% RDF for the first two crops. However, in subsequent years, i.e., IV-rice and IV-wheat, due to a decrease in the residual effect of SSL (applied in III-rice), the amount of chemical fertilizer had to be increased to 70% RDF with SSL (20 Mg ha
−1 SSL + 70% RDF) to obtain similar grain yield to that of 100% RDF. There is a strong relationship between yield attributes and yield, particularly with respect to grain number in the panicle/ear. It was noted that the joint application of SSL with chemical fertilizer treatments increased different yield indicators, such as effective tillers and the weight of 1000 grains, thus producing higher grain yield (
Figure 4). It was found that the use of SSL in RWCS had the potential to substitute half the dose of fertilizers. The yield increment could be explained by the fact that SSL as a source of organic matter contains various nutrients (macro and micro) and provides them to crops slowly after their decomposition [
53]. Thus, improved number of grains per panicle/ear, panicle/ear length, and tillers of rice and wheat were positively correlated with joint application of SSL and chemical fertilizer during both years. The results of the present study are supported by Rehman and Qayyum [
45], who noted that SSL treatment increased the growth and yield of rice and wheat, which might be due to higher uptake of water and nutrients by plants.
Data depicted in
Figure 4 show that joint application of chemical fertilizer and SSL produced significantly higher straw yield than without fertilization (T
0) but was at par with T
1 (100% RDF) in both years. Among all the treatments, T
3 (100% RDF + 30 Mg ha
−1 SSL) had the highest straw yield of the rice crop (8150 and 7896 kg ha
−1) and wheat crop (5695 and 5599 kg ha
−1), respectively, during the course of the experiments. In III-rice, the straw yield of treatments T
2 (100% RDF + 20 Mg ha
−1 SSL), T
3 (100% RDF + 30 Mg ha
−1 SSL), and T
9 (70% RDF + 30 Mg ha
−1 SSL) increased by 4.07, 5.98, and 0.07%, respectively, compared to treatment T
1 where 100% RDF was applied. In the case of IV-rice, treatment T
2 (100% RDF + 20 Mg ha
−1 SSL) and T
3 (100% RDF + 30 Mg ha
−1 SSL) produced 1.10 and 2.64% higher straw yield compared to the T
1. With the III-wheat crop, straw yield of treatment T
2 (20 Mg ha
−1 SSL + 100% RDF), T
3 (30 Mg ha
−1 SSL + 100% RDF) and T
9 (30 Mg ha
−1 SSL + 70% RDF) showed 8.83, 13.18 and 1.58% increments over 100% RDF (T
1), whereas, in the case of IV-wheat, only treatment T
2 (20 Mg ha
−1 SSL + 100% RDF) and T
3 (30 Mg ha
−1 SSL + 100% RDF) showed a positive increment in straw yield over 100% RDF (T
1). Greater leaf chlorophyll contents improve photosynthetic rate, which results in higher crop biomass and yield. The joint application of SSL with chemical fertilizer improves nutrient availability to the plants which improves their root development, the number of tillers, leaves count and ultimately higher straw production. Similar results were reported by Jamil et al. [
49] and Al-Mustafa et al. [
54].
From two years of pooled experimental data, it was found that grain and straw yield of rice and wheat considerably increased or decreased compared to 100% RDF (T
1) (
Figure 5). Application of 30 Mg ha
−1 SSL + 100% RDF (T
3) had maximum enhancement of grain yield in rice (8.1%) over 100% RDF (T
1) followed by the 20 Mg ha
−1 SSL + 100% RDF plot (5.1%). Application of a reduced dose of CF i.e., 50, 60, and 70% of RDF, along with 20 or 30 Mg ha
−1 SSL i.e., T
4 (50% RDF + 20 Mg ha
−1 SSL), T
5 (60% RDF + 20 Mg ha
−1 SSL), T
6 (70% RDF + 20 Mg ha
−1 SSL), T
7 (50% RDF + 30 Mg ha
−1 SSL), T
8 (60% RDF + 30 Mg ha
−1 SSL) and T
9 (70% RDF + 30 Mg ha
−1 SSL) resulted in 15, 10, 2.9, 4.9 1.6 and 0.3% reductions in rice grain yield over T
1, respectively. However, the greatest decrease was seen in the T
0 treatment (72.9%).
Concerning wheat, the highest increase in grain production over 100% RDF (T
1) was recorded in T
3 (30 Mg ha
−1 SSL + 100% RDF; 18.9%) followed by 20 Mg ha
−1 SSL + 100% RDF (T
2), 20 Mg ha
−1 SSL + 70% RDF (T
6), 30 Mg ha
−1 SSL + 60% RDF (T
8; 3.3%) and 30 Mg ha
−1 SSL + 70% RDF (T
9; 4.5%). An almost parallel trend was recorded with respect to the straw yield of rice and wheat. The highest increment in straw yield of rice (4.51%) and wheat (11.3%) over T
1 (100% RDF).was seen in T
3 (30 Mg ha
−1 SSL + 100% RDF). Application of SSL with CF increased the grain and straw of rice and wheat yield percentage compared to 100% RDF due to slow release of nutrients from SSL throughout the period of crop growth, this finding being in accordance with the results of [
22]. Application of any kind of fertilizer resulted in a greater response in wheat crop compared to rice due to different cultivation practices of rice and wheat. Yadav et al. [
55], Gami et al. [
56] and Bhatt et al. [
57] stated that long-term integrated use of manure and fertilizers practiced in RWCS produces higher wheat yield than rice over only chemically fertilized plots.
3.4. Sewage Sludge and Fertilizers Influence the Harvest Index and Test Weight of Rice and Wheat
Data pertaining to HI as affected by the joint application of SSL and fertilizer as shown in
Table 4. Among all the treatments, T
3 (100% RDF + 30 Mg ha
−1 SSL) produced the highest HI in rice (45.00 and 44.67) and wheat crops (47.97 and 47.19) during both years. Significantly lower HI was recorded in T
0 in the rice crop (28.83 and 27.15) and in the wheat crop (38.66 and 36.12) during both years. Latare et al. [
21], stated that an SSL treatment improved HI significantly in wheat but was non-significant in rice. This might be due to additional nutrients available to residual grown wheat from SSL-altered soil.
The data with respect to 1000 grain weight (test weight) of rice and wheat are shown in
Table 4. Among all the treatments, T
3 (100% RDF + 30 Mg ha
−1 SSL) had the highest test weight in the rice (25.88 and 25.80) and wheat crop (33.86 and 33.18) during 2017–2018 and 2018–2019, respectively. In the III-Rice crop, T
2 (100% RDF + 20 Mg ha
−1 SSL) and T
3 (100% RDF + 30 Mg ha
−1 SSL) had 16.61% and 18.97% greater test weights in comparison to T
1 (100% RDF). In the case of the IV-rice crop, T
2 (100% RDF + 20 Mg ha
−1 SSL) and T
3 (100% RDF + 30 Mg ha
−1 SSL) produced, respectively, 12.41% and 13.54% higher test weights over T
1 (100% RDF), whereas, in the case of the III-wheat crop, the test weight in T
2 (100% RDF + 20 Mg ha
−1 SSL) and T
3 (100% RDF + 30 Mg ha
−1 SSL) was 9.10% and 12.99% higher than T
1 (100% RDF), respectively. In the IV-wheat crop, T
2 (20 Mg ha
−1 SSL + 100% RDF) and T
3 (30 Mg ha
−1 SSL + 60% RDF) showed 2.50 and 6.61% higher test weights over 100% RDF (T
1), respectively. The SSL-amended soil favoured vegetative growth, development, and maturity of rice and wheat. This can be explained by optimal uptake of trace, micronutrients, and macronutrients by crop plants that support various biochemical and physiological processes, resulting in higher vigour of seeds. Jamil et al. [
49] reported a significant rise in 1000 grain weight of wheat with the use of SSL compared to control. Barbarick et al. [
58] and Elsokkary et al. [
59] also reported that SSL-based nutrient management improved the productivity of crop plants, including 1000 grain weight.
3.6. Sewage Sludge and Fertilizers Influence the Cadmium, Chromium, Nickel and Lead Concentration (mg kg−1) of Rice and Wheat
The SSL and fertilizer treatments had higher Cd concentration in rice and wheat grain compared to 100% RDF (
Table 6) treatment. In III-Rice, the highest Cd concentration was observed in treatment T
3 (100% RDF + 30 Mg ha
−1 SSL) at 1.27 mg kg
−1, followed by T
9 (70% RDF + 30 Mg ha
−1 SSL) at 1.19 mg kg
−1, and T
8 60% (RDF + 30 Mg ha
−1 SSL) at 1.14 mg kg
−1) which showed 184, 166 and 154% increases over T
1 (100% RDF). An almost similar trend was seen in III-Wheat and the highest Cd concentration was observed in treatment T
3 (100% RDF + 30 Mg ha
−1 SSL) at 1.36 mg kg
−1, followed by T
9 (70% RDF + 30 Mg ha
−1 SSL) at 1.26 mg kg
−1, and T
8 (60% RDF + 30 Mg ha
−1 SSL) at 1.25 mg kg
−1, which were 167, 146 and 144% higher that T
1 (0.51 mg kg
−1). The lowest Cd concentration was seen in T
0 (0.33 mg kg
−1) which was statistically lower than T
1 (100% RDF).
During the 2018–2019 (IV-rice and IV-Wheat) season of the experiment, treatments receiving SSL with CF had significantly higher Cd concentrations then T
1 in grains of IV-rice, and a similar trend was noticed in IV-wheat. In IV-Rice, the Cd concentration was in the order of: T
3 (1.23 mg kg
−1) > T
9 (1.16 mg kg
−1) > T
8 (1.11 mg kg
−1) > T
2 (1.10 mg kg
−1) > T
7 (1.05 mg kg
−1) > T
6 (0.83 mg kg
−1) = T
5 (0.83 mg kg
−1) > T
4 (0.80 mg kg
−1) > T
1 (0.42 mg kg
−1) > T
0 (0.25 mg kg
−1), with respective increases of 195, 178, 166, 163, 153, 99, 99 and 93% over T
1 (0.42 mg kg
−1). In IV-Wheat, the order was: T
3 (167%) > T
9 (150%) > T
8 (148%) > T
2 (145%) > T
7 (141%) > T
6 (88%) > T
5 (85%) >T
4 (74% increase) over T
1 (100% RDF). Overall, the Cd concentration in grain increased with joint application of sewage sludge, i.e., 20 and 30 Mg ha
−1, and full or reduced dose of CF, compared to 100% RDF. This study revealed that Cd concentration was highest (1.36 mg kg
−1) in wheat grain but below the permissible limits of Cd, which are 4 mg kg
−1 and 12 mg kg
−1 in Poland and the Czech Republic, respectively [
64]. Furthermore, the study also found that Cd accumulation in grain did not exceed the phytotoxic threshold level of 5–30 mg kg
−1 [
65]. The Cd concentration was low in rice compared to wheat in the grain. In comparison to wheat, the lower Cd content in rice could be explained due to the submergence condition. Under flooded condition, Cd forms insoluble compounds such as Cd sulfide and/or Cd carbonate which reduce its availability to the rice plants [
66,
67]. Greger [
68], reported that magnification of heavy metals levels in plants is influenced by soil properties, SSL composition, the application rate of SSL, and elemental speciation [
69].
The data pertaining to Cr concentration in grain (
Table 6) showed significantly higher Cr concentration with all combined treatments of SSL with CF compared to RDF. During 2017–2018, the maximum Cr concentration in III-rice was recorded in treatment T
3 (4.90) followed by T
9 (4.85) and T
8 (4.79), whereas in III-Wheat it was in treatment T
3 (4.49) followed by T
9 (4.34) and T
2 (4.22), with a respective significant increase of 148, 146 and 143% in III-Rice and 156, 148 and 141% in III-wheat compared to 100% RDF (T
1). During 2018–2019 (IV-rice and IV-Wheat), the maximum Cr concentration in IV-Rice (4.11 mg kg
−1) and IV-wheat (3.55 mg kg
−1) was recorded in T
3 (30 Mg ha
−1 SSL). The application of 20 and 30 Mg ha
−1 SSL with full or reduced doses of CF (T
2, T
3, T
4, T
5, T
6, T
7, T
8 and T
9) significantly increased the Cr concentration in grain by 2.43, 2.86, 2.00, 2.06, 2.11, 2.37, 2.46 and 2.76 times in IV-Rice and 2.55, 2.79, 1.96, 1.99, 2.11, 2.24, 2.37 and 2.73 times in IV-Wheat, respectively, over 100% RDF (T
1). The phytotoxic limit of Cr is 5–30 mg kg
−1 [
65]. This result indicates that Cr concentration in grain was within the acceptable limit and did not cross the phytotoxic threshold level.
The results show that the Ni concentration in III-rice varied from 7.65 to 19.00 mg kg
−1, whereas, in III-wheat it ranged between 7.93 to 17.31 mg kg
−1 (
Table 7). During 2017–2018, the maximum Ni concentration in III-rice (19.00 mg kg
−1) and III-wheat (17.31 mg kg
−1) was recorded in treatment T
3 (100% RDF + 30 Mg ha
−1 SSL). The application of 20 and 30 Mg ha
−1 SSL along with a full dose or reduced dose of CF significantly increased the Ni concentration in grains of III-rice and III-wheat compared to 100% RDF (T
1). During 2018–2019, the Ni concentration in grain ranged between 7.35 to 5.48, and 6.28 to 14.35 mg kg
−1, in IV-rice and IV-wheat, respectively. The greatest Ni concentration in IV-Rice (15.48 mg kg
−1) and IV-wheat (14.35 mg kg
−1) was recorded in T
3 (100% RDF + 30 Mg ha
−1 SSL). The application of 30 Mg ha
−1 SSL along with a reduced dose of CF (50, 60, 70% of RDF), i.e., T
7, T
8 and T
9 resulted in significant increases in Ni concentration in grains by 45, 48 and 61% in IV-rice, respectively, over 100% RDF (T
1), whereas in IV-wheat, these treatments were statistically at par with T
1 (100% RDF). All the treatments amended with 20 Mg ha
−1 SSL along with a reduced dose of CF (50, 60, 70 of RDF), i.e., T
4, T
5 and T
6, did not show a significant increase of Ni in grain compared to 100% RDF in both crops (IV-rice and IV-wheat). The Ni concentration was below the phytotoxic limit of 10–100 mg kg
−1 as in [
65]. Out of the various treatments (
Table 7), T
3 (100% RDF + 30 Mg ha
−1 SSL) had the highest Pb concentration in III-rice grain (1.99) and III-wheat grain (1.94). The joint application of 20 and 30 Mg ha
−1 SSL and full dose or reduced doses CF (T
2, T
3, T
4, T
5, T
6, T
7, T
8 and T
9) in III-rice significantly increased the Pb concentration in grain by 1.89, 2.34, 1.52, 1.57, 1.65, 1.77, 1.95 and 2.25 times, respectively, compared to 100% RDF. The corresponding increases of Pb concentration in III-wheat were 2.53, 2.88, 1.83, 1.91, 2.04, 2.08, 2.14 and 2.77 times.
During 2018–2019, (IV-rice and IV-wheat), all the treatments of SSL (T
3–T
9) were significantly higher in Pb concentration compared to 100% RDF. The Pb concentration in grain ranged from 0.40 to 1.81 and 0.37 to 1.53 mg kg
−1 in IV-rice and IV-wheat, respectively. The highest Pb concentrations in IV-Rice (1.81 mg kg
−1) and IV-Wheat (1.53 mg kg
−1) were recorded in T
3 (30 Mg ha
−1 SSL). Treatments T
2, T
3, T
4, T
5, T
6, T
7, T
8 and T
9 when compared with RDF had corresponding increases of 2.24, 2.87, 1.87, 1.89, 2.03, 2.13 and 2.75 times in IV-rice and 1.95, 2.57, 1.58, 1.67, 1.67, 1.94, 1.96 and 2 times in IV-wheat. The lowest Pb concentration was recorded in T
0 during the course of the experiment. The present investigation revealed that Pb (highest, 1.99 mg kg
−1 in III-rice) in rice and wheat grain were below phytotoxic limits (30–300 mg kg
−1) as outlined by [
65]. Singh and Agrawal [
70] and Eid et al. [
71] reported an increase in heavy metal concentration in the areal parts of barley by application of SSL. Zoubi et al. [
72] reported similar findings.
3.7. Total Heavy Metal Content in Post-Harvest Soil after Completion of the Experiment
The total Cd, Cr, Ni and Pb content in soils after the termination of the experiment ranged from 0.44 to 2.53, 2.25 to 9.26, 7.98 to 21.23 and 4.45 to 27.36 mg kg
−1, respectively (
Figure 6). Among all the treatments, T
3 (100% RDF + 30 Mg ha
−1 SSL) had the highest total Cd, Cr, Ni and Pb after harvest of IV-wheat. The treatments that received 30 SSL Mg ha
−1 (T
3, T
7, T
8 and T
9) increased the total Cd content by 5.75, 3.2 3.3 and 3.6 times, respectively over T
1, whereas, treatments T
2, T
4, T
5 and T
6 that received a lower dose (20 SSL Mg ha
−1) increased by 3.2, 2.9, 2.9 and 3.0 times, respectively. However, total Cr content soil after harvest of the IV-wheat crop showed a declining trend in the order of T
3 (9.26) > T
9 (9.15 mg kg
−1) > T
8 (8.88 mg kg
−1) > T
7 (8.45 mg kg
−1) > T
2 (7.77 mg kg
−1) > T
6 (7.89 mg kg
−1) > T
5 (7.69 mg kg
−1) > T
4 (7.22 mg kg
−1).
These data were statistically similar to one another but significantly greater T
1 (2.59 mg kg
−1). The total Ni content in post-harvest soils significantly increased due to the application of SSL. The 100% RDF treatment, i.e., T
1 (10.25 mg kg
−1) was statistically at par with all other treatments except T
2 (18.0 mg kg
−1), T
3 (21.23 mg kg
−1) and T
9 (18.65 mg kg
−1) which had the highest content of Ni in the post-harvest soil. Treatments T
3 (100% RDF + 30 Mg ha
−1 SSL), T
7 (50% RDF + 30 Mg ha
−1 SSL), T
8 (60% RDF + 30 Mg ha
−1 SSL) and T
9 (70% RDF + 30 Mg ha
−1 SSL) had increased Pb content by 3.32, 3.09 3.08 and 2.98 times, respectively, over T
1 (100% RDF), whereas in treatments T
2 (100% RDF + 20 Mg ha
−1 SSL), T
4 (50% RDF + 20 Mg ha
−1 SSL), T
5 (60% RDF + 20 Mg ha
−1 SSL) and T
6 (70% RDF + 20 Mg ha
−1 SSL) with lower dose of SSL (20 Mg ha
−1), the respective increases were 2.66, 2.55, 2.58 and 2.45 times. The total heavy metal contents in soil were within the maximum permissible limits (MPL) with respect to the limits [
64] for India and for Poland and the European Union [
28] (
Figure 6). The results indicate that total heavy metal contents in soil were within MPL even after applying the highest dose of SSL (30 Mg ha
−1) with 100% RDF.